In the Sonic the Hedgehog games and most cartoon adaptations, Dr "Eggman" Robotnik is villainous, but with a highly affable and clownish demeanor, and in some cases leans into Anti-Villain territory. Robotnik of Sonic SatAM and to a lesser extent Sonic Underground, however, is a monstrous (and far less humorous) dictator that not only has taken over most of the planet but thrives almost lustfully on having any remaining civilians painfullyroboticized. This depiction is drifted in and out for both comic adaptations (although they refer to his more petty, comical personality a lot more).
In the book Cranberry Christmas, Cyrus Grape is a curmudgeonly old man who refuses to let anyone skate on his pond, but gets his comeuppance when Mr. Whiskers finds a deed that proves the lake is actually on his property. In the animated special, Cyrus is a much more active antagonist, sneaking around and messing up Mr. Whiskers's house in order to keep Mr. Whiskers from finding that deed (whereas in the book he had no idea it existed).
Transformers Animated actually did this to the character Waspinator from Beast Wars. While Beast Wars Waspinator is portrayed as the lovable Butt Monkey who does nothing but get kicked around by other characters (though he does manage to injure the occasional Maximal, usually not by accident), Animated Waspinator, now renamed Wasp, is downright terrifying, and wants to get revenge on everyone who abused him.
Klarion the Witch Boy, whose portrayal in the comics generally ranges from an annoying troublemaker (Jack Kirby's version) to a well-meaning anti-hero (Grant Morrison's version), is much more solidly on the side of the black hats in Young Justice.
Also played straight with L-Ron. In the comics, he's a sidekick to the Justice League International, while in the show he's Despero's assistant.
Tublat the gorilla from Tarzan by Edgar Rice Burroughs. In Disney's The Legend of Tarzan, his character is merged rather confusingly with another, Kerchak. Since Disney decided to make their version of Kerchak (who is ironically more similar to Burroughs's Tublat in personality) more sympathetic, as a consequence they ended up making their version of Tublat more sinister, like the novel's Kerchak.
Word of God says that had the show continued, she would have evolved into her usual anti-heroic persona.
Also inverted with Frederick Foswell. In the original comics he was the crime boss known as The Big Man and after his release tried returning to crime before going up against the Kingpin, making a Heel-Face Turn, and ultimately sacrificing himself to save J. Jonah Jameson. In the show he's a journalist on the up and up from the beginning.
Ricochet is a member of the Enforcers (Fancy Dan) rather than a teen vigilante like in the comics.
Anubis is a villain in the TV show Mummies Alive!, when he was actually a good god in Egyptian Mythology who guarded and protected the dead. Set is also seen with Anubis, while Set disowned him in the myths for siding with Horus.
Ammit, on the other hand, is portrayed as a pet of the Big Bad. In Egyptian mythology she was a neutral enforcer of order and punisher of evil, although this quality made her feared by the ancient Egyptians.
The Street Fighter animated series made Zangief into one of M. Bison's lackeys, despite the fact that Zangief actually opposed Shadaloo in the games.
Colossus and Gambit were members of Magneto's Acolytes in X-Men: Evolution, despite being actual members of the X-Men in the comics. They eventually pulled a Heel-Face Turn and were seen as part of the team in the epilogue.
Domino is a member of the X-Force and X-Men in the comics, but is depicted as a terrorist and member of the Brotherhood of Mutants in the show, basically becoming Mystique in all but name and powers as Mystique herself is Magneto's Dragon.
Multiple Man is a member of Mr. Sinister's Marauders, despite being a main character in X-Factor since the 90's.
Likewise, the Stepford Cuckoos are shown as villainous members of the Hellfire Club, despite being students at the Xavier Institute in the comics.
Psylocke assists the Brotherhood in one episode, but she's shown to be a reluctant recruit who only helps out the group because she owes Quicksilver a favor.
Mercury, another member of the Acolytes, was a member of the New X-Men in the comics.
In the comics, Scarlet Witch and Quicksilver abandoned Magneto very quickly and joined The Avengers. In the show, Quicksilver is still a member of the Brotherhood, while Scarlet Witch is loyal to her dad. It isn't until the finale that she finally realizes what a monster Magneto is and turns against him.
Mags himself: in the comics, he's a Well-Intentioned Extremist or an Anti-Hero depending on the decade. He was last wa-ha-ha evil in The Seventies, and the last time he was an enemy was done in such an Out-of-Character Moment that it was Retconned into being someone else immediately, making a 1993 storyline the last time we saw him as anything but his normal portrayal (half the team wants to trust him, the other half says "yeah, but you don't know how bad he was when he was bad," and his Wild Card moments don't make anybody any more comfortable.) and it's not like nobody provoked him then*
Of course, he gave 'em plenty of reason to think they had to strike first... it's complicated.
WATXM Magneto appears to be similar to comic Magneto but at heart is as monstrous as it gets, more like his sixties/Morrison/Ultimate incarnations.
Emma Frost. Like Mags, she used to be one hell of a foe (even being Big Bad of The New Mutants for a time) but comic fans know that that was a long time ago, at least in the main Marvel Universe. In this one she's The Mole and still the White Queen of the Hellfire Club. However, in the finale she sacrifices life to contain the Phoenix.
The Phoenix. This is far from the first adaptation to do so, but it's worth mentioning that in the comics, Jean as Phoenix was good but Anti-Hero-ish, had to resist darker impulses but stayed in control (she was actually Phoenix for quite some time), and even saved the universe. It took the Hellfire Club's interference to cause her to become Dark Phoenix. This version uses The Theme Park Version where the Phoenix is a 100% Bad Thing. Of course, the Hellfire Club was trying to control the Phoenix in this version, but it wasn't quite the same as Jason Wyngarde and Emma Frost putting her under More Than Mind Control and pretty much breaking down her self-control bit by bit until we get a monster.
Morrigan in the Darkstalkers cartoon. In the games, she is just having fun with no regard for the rest of the cast, in the show, she's Pyron's minion. The series finale implies she becomes closer to how she is in the games if a season 2 ever came. Also, Anakaris, Bishamon, and to some extent Demitri were victims of this.
The Falcon and Doc Samson appear as part of Code Red, a team of government-sponsored superheroes who act in opposition to the Avengers. In the comics, the Falcon is Captain America's sidekick and a longtime member of the Avengers himself, while Doc Samson is an ally of the Hulk. Partially justified though, since it turns out they were brainwashed by the Red Skull. (And both of them have had notable Brainwashed and Crazy stories in the comics; in Falcon's case at the hands of the Skull.)
In The Railway Series novels, Diesel only returned to Sodor once in the individual story "Thomas and the Evil Diesel" where he redeemed himself and was given good word to come back. In the Thomas And Friends series, Diesel made recurring returns to Sodor and eventually became a permanent resident, though he ultimately proved as nasty as before, usually acting as the key antagonistic engine and pulling cruel pranks. Similarly to the novel version though, he is given some sympathetic moments.
Reversed for Bulgy, a bus who disliked railways and tried to steal customers from the trains through lying that he accepted rail tickets. In the books, he is punished by being converted into a henhouse. While this is followed in his first appearance in the TV series, he is later repaired, changed into a vegetable stand, and softens towards the other characters.
The animated movie Heidi's Song is a curious example of this, as it not only makes Fraulein Rottenmeier much more villainous and scary, but also turns Sebastian the butler (in the book a Servile Snarker but very much a kind man) into her Dragon — but utterly reverses it when it comes to Tinette the maid, who in the book is a haughty and snooty woman whom Heidi is slightly afraid of but in the movie is a sweet and sympathetic person. Possibly the shift was done so the movie wouldn't have two female villains.
In the Funny Animal adaptation The Legends Of Treasure Island Long John Silver is a more straight up Laughably Evil villain and mostly void of the sympathetic Affably Evil facets of his novel counterpart (and most other variations of). Perhaps most notably, his fatherly role with Jim is completely gone and for the most part, he would love nothing better than to just send the boy down the plank, or worse.
For most of the Super Friends series, Bizarro is depicted as a clear villain who has murderous designs on the super heroes. However, the final season depicts him faithfully from the comics as a well meaning bumbler.
While the original comic book incarnation of Teenage Mutant Ninja Turtles' Karai has interests that occasionally pit her against the turtles, she is unambiguously their ally. This has changed in the 2003 and 2012 cartoon adaptations, where she has been made into the Shredder's daughter and subordinate. While she will at times fight alongside the turtles, her divided loyalties result in periods where she is wholeheartedly against them.
The 80's cartoon is notable for being the only version to portray the character of Leatherhead as truly villainous, as opposed toallotherversions where he is an ally of the Turtles, and any time he fights them in those continuities is because of him being either Not Himself or manipulated into doing it by another antagonist.
Zig-zagged and parodied in Teen Titans Go! with Terra. The original Teen Titans made her an example of Adaptational Heroism. In the episode "Terra-ized", she has actions similar to her comic book counterpart; and openly tries to seduce Beast Boy in order to get sensitive information on the Titans. Only Robin and Raven suspect her of villainy, while Cyborg and Starfire are not convinced despite Terra trying to bring them down every scene she's in. When Beast Boy tries to return her advances, she drops all pretense and decides to fight the Titans for the information she needs.
Sunset Shimmer counts too. Her toy bio doesn't give any hint she's remotely malicious.
Brainy in The Smurfs episode "King Smurf" became the titular character, whereas in the original comic book version he was a contender for the role of the village leader who was outvoted in favor of the Smurf who would become King Smurf.