L who was was specifically designed to be unattractive. His appearance and behaviour were designed to contrast Light, who is Tall, Dark and Handsome.
Yuuko Ichihara of XXX Holic. Most color illustrations depict the rest of the main cast as these, too. All the main characters have pasty skin and, sans Kohane, dark hair in the manga, due to the way the art was stylized. The anime and official crossover illustrations depict both Doumeki and Himawari with healthier complexions, but Watanuki and Yuuko both remain very pale.
Sunako from The Wallflower. The boys in charge of making her into a lady initially mistake her for Sadako thanks to the general aura of creepy she constantly emanates.
Kuromitsu, the beautiful, immortal vampire from Kurozuka.
Sawako from Kimi ni Todoke, whose creepy looks have had her nicknamed Sadako. She's actually very nice, very naive, and really lonely (since her looks and her (mostly untrue) reputation tends to scare off potential friends).
Orochimaru of Naruto goes beyond simply having pale skin — his is flat-out white, paired with black hair. Sai, Itachi, and Sasuke are less pale, but they all contrast with Naruto, who is blond-haired and well-tanned. More heroic examples are Hinata and Neji Hyuga, although Neji starts out as a fatalistic Arrogant Kung-Fu Guy and Hinata is described as "gloomy" by Naruto (although he still has a positive opinion of her).
Saki Hanajima from Fruits Basket, complete with creepy goth tendencies and an unflattering reputation. Her younger brother Megumi is one of these too, and he's arguably even creepier than she is. Rin and Akito, both Broken Birds, also fit this trope.
Momoko of Saki. This, combined with her ~su Verbal Tic, her power to disappear from sight, and the black smoke effect used to portray those powers, makes her seem like a ghost.
Re-l Mayer from Ergo Proxy, whose pure white skin, pitch black hair, and liberal amounts of blue eyeshadow make her rather...striking.
Ulquiorra Schiffer has bone-white skin and jet black hair and his colouring stands out from all other characters around him as a result. He's a symbol of nihilism and his lifeless pallor is part of his theme of not truly understand what it means to live.
Zaraki's idol Yachiru, the very first Kenpachi and founder of the 11th Division, was an Ax-CrazyBlood Knight whose viciousness in battle was something Zaraki aspired to emulate. In battle, her long hair flowed free and her face would take on an eerie expression that would switch from unnaturally detached to psychopathic depending on how the fight was progressing. However, in later years she became the 4th Division Combat Medic Captain Unohana, famed for her beauty in-universe and viewed as the perfect Yamato Nadeshiko, and who always kept her hair neatly bound. Word of God stated Unohana was Soul Society's most beautiful woman and that he wanted there to be a shocking contrast between the two faces of her personality.
D.Gray-Man has two heroic examples: Krory and Miranda.
Death the Kid from Soul Eater. He's a nice enough if eccentric chap, but he does have black-and-white hair, slightly creepy yellow eyes, and comes across as more eerie than is the norm even for this series when he fights 'properly' or talks about gods, life, and death. And that's before you factor in his temporary insanity.
Emma from Victorian Romance Emma gives off vibes like this to those around her, which led a few men to court her, but is often considered aloof by her peers.
Shiki from Togainu no Chi has skin that's practically white and black hair. Were it not for his red eyes, in fact, he would have a very monochromatic appearance since he wears black all the time.
Zeref from Fairy Tail, despite the fact that he's seemingly spent a very long period of time living outdoors in an area with a tropical climate, and ought to be well tanned.
Homura Akemi from Puella Magi Madoka Magica, notable compares on other casts who have healthy tan or blush. She's so pale her skin tone is closer to gray than mere white. Justified by her half a year hospitalization.
Mei Misaki from Another. We learn fairly quickly that she's rather nice.
The titular Blue Exorcist, OkumuraRin is this trope. More so in the manga than anime version, as the anime gave him some colour in his skin and changed his dark black hair into a navy blue. He also subverts the traditional not The Big Guy role as he's the strongest of the main cast.
K's Fushimi Saruhiko is extremely pale, bordering on gray actually, and has the dark hair to match. Misaki even comments on how unhealthy pale he is in a side story featuring their early life together.
Haruka's alternate self, Konoha, becomes this when he is possessed by the Wide-Eyes Snake and transformed into Kuroha◊, the series' main antagonist. Kuroha, in contrast to the above, is much more in-keeping - to the point that his arrival in any given adaptation is almost always signalled by a shot of his face with Hidden Eyes, or a Slasher Smile (or both).
Death and Dream of the Endless, though the former is a much cheerier Perky Goth to her brother's somber disposition. The Endless can change their appearance; Dream appears African to one of his Girlfriends.
Desire and Despair.
Averted with Delirium and Destruction. The former has pale skin but mercurial rainbow hair, while the latter is a hale looking redhead. With Destiny you can't really tell because of the hood.
The Bride of Nine Spiders from Immortal Iron Fist. Fittingly, her main power is the ability to summon hordes of spiders.
Due to his blood disease Morbius was pale even before the scientific accident that transformed him into a living vampire, but after it it turned him outright creepy. The lack of melanin in his skin makes it pure white, while his hair has remained completely black.
H'el, the main antagonist from H'el on Earth. Flashbacks reveal that he wasn't always so pale, but how he got his current complexion is a mystery even to him.
Moon from Pocket God is a goth girl who is fascinated by death and likes doing fatal stunts for the thrill, knowing that she will always resurrect if she dies. Her paleness is especially noticeable because the other pygmies have dark skin.
Laura Kinney aka X-23 crosses this over with Raven Hair, Ivory Skin. She's most commonly drawn with black hair and very fair skin, and is often depicted as a goth. One of the other prostitutes in NYX specifically calls her "the creepy one" since no one knows her name, which certainly qualifies her for the "eerie" part.
Fairy Tales and Folklore
"Snow White": Back in the day, unnatural paleness was the epitome of feminine beauty, since tanned skin was associated with commoners who worked outside all day. Snow White looks gorgeous after her death, but the paleness=corpse=unnatural association wasn't present in the original story.
The legend of the Yuki-onna or Snow Lady in Japanese mythos. Exceptionally pale and beautiful, but her eyes can be terrifying. She may also lack feet.
The Stoker family in Stoker, and particularly India Stoker.
In Waltz with Bashir, the director portrays his ex-girlfriend, who dumped him the same week he shipped out, as one of these. He has fantasies of her as a ghostly presence on the battlefield. In an interview, the director stated that his wife objected to how attractive he made her in the film.
Heck, every character in the film could fit this trope. Possibly intentional? The four main girls were particularly creepy whenever they stood in a row and just stared someone down.
Elvira, Mistress of the Dark fits this trope to a tee. Then she turns out to be extraordinarily spiteful, cruel, and manipulative (far from the angelic image she's remembered as), so she also fits into the evil, dark-haired, pale-skinned group.
Kill List has Fiona, Gal's new girlfriend. There's something distinctly off about her and her appearance and strange actions during Jay's dinner party are one of the first major hints that something is very wrong here.
Louis of Interview with the Vampire, as mentioned below under Literature. The film both increased it by letting us see his veins through his skin and generally putting us outside his own narration, and decreased it by turning his jet-black hair brown. It also turned Armand into this, where he was a cherubic young redhead (though no less creepy) in the books.
It's safe to assume that Sirius's skin lost its waxy look after he'd been out of Azkaban for a while. Considering he was also dirty and emaciated at the time, it was probably caused by his poor health more than actual paleness.
Also, Bellatrix, who, in the movies, is played by the pictured Helena Bonham-Carter. And the rest of the Black family except Narcissa, who looks more like her husband for some reason.
Tom Riddle was one in his youth, laminated by Frank Dillane and Hero Fiennes-Tiffin's portrayal of him in Harry Potter and the Half-Blood Prince, as a sixteen-year old Tom and eleven-year old Tom respectively. Both actors crank Tom Riddle's creepiness Up to Eleven. This, in turn, creeps Harry out, as he looks a bit like him. Rowling loves this trope.
Isa, from Only Echoes Remain, is preternaturally pale and beautiful, with extremely long and lustrous ebony hair. Despite her protests, the look does suit her, as she is a spirit being specifically designed as a (relatively minor) manifestation of darkness and death.
Gregor Vorbarra from the Vorkosigan Saga is described as being like this - as well as being tall and thin and dressed in dark clothing - so it shouldn't be surprising that he's The Emperor of a multi-planetary, extremely militaristic empire. Except that he's also one of the good guys.
Most of Miles Vorkosigan's love interests fit this trope too, especially Elena and Elli.
House Raith of the White Court in The Dresden Files - a clan of psychic vampires that feed on lust and all look like this.
Unless, of course, you know that the gorgeous person with black hair and pale skin that you can't resist is a White Court vampire who not only eats emotions but the energy that, in-universe, composes souls—and that he or she can drain away your soul while feeding. ALL of it, if he or she is hungry enough. To the point where you won't merely die...the mental/emotional/spiritual you will cease to exist. Forever. And, because the sex is so outstanding, you won't even want to fight back.
Juliet Salazar from Mike Carey's Felix Castor series, who has black hair, "black-on-black" eyes, and pure white skin: "the undiluted white of snow or bone rather than the muddy pink-beige mix that passes for white according to normal labelling conventions." Justified in her case, as she's a demon from Hell whose body isn't, technically speaking, an actual body. And in something of a subversion, she's not necessarily an evil demon from Hell, when she chooses not to be.
Ashara Dayne from A Song of Ice and Fire is almost always described as a "haunting" woman with dark hair and violet eyes.
Littlefinger apparently thinks he is one of these, as his only response when Tyrion threatens to send him to the Night's Watch, was to complain that the black uniform would only enhance this.
Heleth from Douglas Hill's ColSec Trilogy is an Eerie Pale-Skinned Brunette with facial tattoos. Justified in that she was raised underground (the tattoos help camouflage her in shadows). And she sunburns badly.
Definitely on the Dark Is Not Evil side of this trope: Stephen Maturin, co-protagonist of the Aubrey-Maturin series. His hair is black, of course, and his skin tone is almost invariably described as "pale" or "sallow".
Emily of New Moon has very pale skin (to the point that, especially when she's a child, most people who meet her assume she's delicate and will likely die of tuberculosis) and black hair. It contributes to most people seeing her as a borderline Creepy Child.
In The Count of Monte Cristo, Edmund Dantes is one of these, having dark hair and extremely pale skin. This is called attention to on several occasions, in which, as the Count, he's described as handsome but with an unsettlingly pale skin tone. The narrator explains that the years he spent in prison made Dantes very pale and prevented him from ever returning to his original tan skin tone.
The title character of Maledicte is an extremely pale, dark-haired, dark-eyed young woman disguised as a man... who also happens to be an amalgam of human and vengeance god. An unusual example, in that Mal, thanks to obsessive training and superpowers, actually is a top-notch physical fighter.
In Doctrine of Labyrinths, Kolkhis has black hair and very pale, bluish skin that makes her "look like the world's most beautiful corpse." She's also the go-to person if you want an assassination in the city of Melusine, and is in league with a blood witch. Vincent looks remarkably like her, and has an unsettling tendency to get distracted by ghosts in the middle of conversations.
Both Coira and Arpazia in the Snow White and the Seven Dwarfs retelling White as Snow alternate between this and Raven Hair, Ivory Skin depending on how creepy they are at the moment. Both women are acknowledged to be very beautiful—Arpazia before she somehow becomes a thirty-year-old crone and Coira after she turns eighteen and comes into her own—but the mother's flares of temper and the daughter's talent for complete stillness and silence frighten people to the point that their beauty almost isn't worth it.
Louis of the Vampire Chronicles has jet-black hair and piercing green eyes, and his skin became white with the transformation into a vampire. He's the narrator of the first book, and the narrator of most of the rest has a big soft spot for him, so he tends to come off as more pitiable than creepy to the reader, but in-universe he's certainly this— especially to mortals.
Belinda Contague from the Garrett, P.I. novels plays up this image to make herself more intimidating as the capa of the TunFaire mob.
Willow at the end of season 6. Justified in that, by that point, she's become completely taken over by grief, revenge lust, and black magic. She gets better.
Drusilla - a Mad Oracle who Angelus put through every variation on Break the Cutie before making her immortal so she'd suffer forever. This doesn't stop her from being as dangerous as the rest of the Fanged Four.
WWE Superstar Mark Callaway, aka The Undertaker (although his natural hair color is actually red), as well as his manager, Paul Bearer. Even after Taker changed his gimmick to a Badass Biker, he's still noticeably pale. His manager Paul Bearer matched this description when he wore face paint.
Zoe Graystone from Caprica has very dark (nearly-black) hair and very light (as close to white as possible without albinism) skin. Particularly noticeable in the ads, in which she is stark-naked and holding a bright-red apple.
The loyal warlock Merlin and the king's ward Morgana, from the BBC's Merlin.
Though Morgana is a better fit for this trope than Merlin, since she's definitely paler-skinned (Merlin doesn't really have that "ghostly" complexion), as well as conveniently turning into a near-psychopathic villainess hellbent on dramatic angst and sorcerous revenge.
Red Riding Hood, better known as Red, having dark hair in Once Upon a Time is a contrast from the original story book version. The change makes sense, because Red is also The Big Bad Wolf that has been terrorizing the town.
Kenzi from Lost Girl is very pale, has long, black hair, and bright blue eyes. Not very "eerie" as much as "comical", though.
The Ninth Doctor. The actor dyed his hair black to invoke this trope. Notably, his most basic personality is Northern and chirpy, so the eerie appearance reminds the audience that he isn't human at all.
Gerard Way of My Chemical Romance has gone through phases of this, with dyed black hair and his natural white-boy-ness. However, he's also gone through a white-headed goth Sgt. Pepper phase, a sassy atomic-redheaded phase, and a brief blond Ray-Ban hipster-looking phase sometime in 2012. His natural color is actually a pretty normal brown.
Tarja Turunen, Amy Lee, Sharon den Adel, Vibeke Stene, Manuela Kraller, Anette Olzon... Gothic and symphonic metal is rife with this trope.
The default appearance of the ScreamQueens, though as a goth, Daffney's appearance is always subject to change. Prior to the team, WCW often used Daffney as the crazy screaming obsessive but also put her in fanservice roles too. MsChif more so enforced the trope just through raw abrasiveness. Draculletta and White Magic, Wrestlicious's Ghouls Gone Wild, are an even straighter case.
Due to flaws in various implants, all Raven Guards have dark hair and pale skin, regardless of what they looked like pre-surgery.
Dark Elves in Warhammer Fantasy are almost all pale and black-haired, though no actual reason is given. Perhaps that was just a major dominant trait among the Nagarytheans.
Nothing in official books, but various pieces of fluff and the occasional Word of God in articles and video-game material state that, yes, Nagarytheans tended towards this aspect. That, and millennia of using dark magic probably hasn't helped matters any...
Moon elves, or Silver elves, in Forgotten Realms usually have black to blue hair and pale to icy-blue skin. At least one novel even lampshaded that the subrace visually is a perfect contrast to Dark-Skinned Blond drow. They look the weirdest of whole elvenkind (except Avariel), but tend to be the most human-like mentally (approachable, curious, and active) and the least decadent.
Ubiquitous in Old World of Darkness with its Gothic aesthetic design. Open a rule book and you will see this trope.
Despite being The Ingenue, Christine Daae in Andrew Lloyd Webber's version of The Phantom of the Opera is sometimes (depending on the actress) played as this, though, in her case, it's mostly to make her look fragile and ethereal◊. In just as many cases, it's subverted by her having a fresh, lively, pink complexion to go with her dark hair, and a few actresses have simply been too dark to even come close to this trope.
The Phantom himself looks like one of these◊ until it turns out his "hair" is actually a wig, and all he really has is a few scraggly wisps of graying brownish hair on an otherwise bald head.
His father, on the other hand, universally falls under this trope.
Laurence Olivier played Shakespeare's Richard III as one of these onstage◊; when he recreated his performance for film, the makeup was toned down and Richard's skin tone was Olivier's own. (Ironically, the real Richard was, according to his surviving portraits, of middling complexion and with light brown hair.)
Soren from Fire Emblem 9 and 10. He's one of the protagonists, but his cynicism and utter lack of idealism occasionally puts off his allies.
Noticeably, Karla of Fire Emblem 7 is the only (female) ally with black hair in the entire game. Mind, this is a series with a tradition of having at least thirty-odd characters on the allies' side alone, and they are all very pale. Upon supporting, her personality is revealed to be an equal mix of Cloud Cuckoo Lander and Lady of War. Strangely for female characters in this trope, she is an undefeated fighter known as the Princess of Swords as well as The Rival to Bartrethe Fighter, and there are absolutely no allusions to her being sickly or weak, though she does die of an illness years after the game ends. In the previous game, her daughter Fir continues the trait of having dark hair along with a few others—though, for some strange reason, Fir's hair is purple.
FE7's Morphs, artificial humans made by the Big Bad, also fall under this.
Viola Cadaverini from the Ace Attorney series. She's meant to be creepy and sickly looking, and it works.
Higashizawa Youdai of The World Ends with You is, considering the rarity of even Big Guys crossing over with this trope, most likely the only Brute example of a Pale-Skinned Brunette in existence.
There's another example and that is Shiki's true self.
Ashei from The Legend of Zelda: Twilight Princess fits this trope physically, with her black braided hair and almost paper-white skin (complete with under-eye dark circles). She's one of the good guys, however.
More like Eerie Pale-Skinned Dark Redhead: Elaine Marley-Threepwood from Tales of Monkey Island, from the time that she willingly becomes LeChuck's demon bride up to the time that Guybrush manages to shrink La Esponja Grande.
Taira no Yukiri from Six Rules's Raven Hair, Ivory Skin beauty turns into this when she is revealed to be a cold-hearted Creepy Child who has been planning the death of the protagonist since the beginning. And she's ten years old.
Phase (Ayla Goodkind) at the Super Hero School Whateley Academy in the Whateley Universe. Her hair is jet-black (it was a sandy-blond back when she was a boy, before she mutated). She's quite pale (some wavelength of light may be passing through her). She's also very rich and highly educated, which fits the trope too. But she's one of the good guys. A lot of mutants don't believe that, because her family are the most notorious mutant-haters anywhere.
Mai and Jun of Avatar: The Last Airbender. And, ahem, the entire freaking Fire Nation royal family. Toph Beifong also appears as this when Aang first sees her in a mysterious vision, but when he actually meets her, she turns out to be a tomboyish and non-eerie Little Miss Badass.
Kevin from Ben 10 starts out this way and is quite psychotic. When he joins the team in the sequel, his skin tone is almost the same as the Tennysons.
Shego from Kim Possible was designed with this in mind. Her green highlights make her seem poisonous. Oddly (given the suggestion above), she's often seen on a beach, or a tanning bed, with no apparent effects; maybe she wants to differentiate herself from her heroic brothers who follow a similar scheme.