Tsugumi of Ever17 is straddling the line between this and kuudere and it's towards everyone except Coco. And Sara, but she ignores her anyway. Obviously, she mellows by the end. Harsh, uses violence, (punches Takeshi at least once) cold shoulder (default. She doesn't answer meaningless questions in her own words) and also the smirk! Actually, she comes off as a bit of a jerkass a lot of the time so they gave her a morality pet before letting her officially act dere towards Takeshi.
Riho towards Shinichi in Deardrops. In her route, it is revealed that she'd been impressed with how he managed to dedicate his life to music and play in a professional orchestra in Germany and was disappointed and angry at him for squandering that chance and returning to Japan.
Hiroki in Canvas 2 is constantly described as a 'contrarian.' On the heroine side of things, Tomoki really tries but is too easily distracted to keep it up.
Tohno Akiha in Tsukihime is this, but being the Ojou, she shows her tsun-tsun side far more often outside her own route and dips into outright Yandere in Kohaku's, thanks to a partial possession by an evil ghost and her own demon blood getting riled. Interestingly enough, Shiki himself is a pretty clear tsundere, but only for Arcueid. He even says himself that he's nice to everyone else.
White Len in Melty Blood for Shiki Nanaya, whom she summoned as a TATARI avatar, mirroring (black) Len's dere-ness for Shiki Tohno.
As pictured on the main page: Rin Tohsaka in Fate/stay night. She's heavily on the tsun side in "Fate"; it's in "Unlimited Blade Works", where she's the main love interest, that her dere side comes out. In the last scenario, "Heaven's Feel", she again plays Worthy Opponent-turns-The Lancer role (considering her servant), but she's still very Tsundere. The focus of it just shifts from Shirou to her sister, Sakura. In fact, in some ways, HF is where her Tsundere nature (and the reasons behind it) is most obvious (especially at the end). A perfect example (which made it into the anime) is the scene where she goes from trying to blast Shirou senseless to tending his Rider-inflicted wounds in the space of a few minutes.
In Fate/kaleid liner PRISMA☆ILLYA, this Rin is set an Alternate Universe and yet this trope applies rather hard to her there. In Fate/EXTRA, the lady is not the same one we know of... and yet she is a Tsundere, through and through. If the name Rin Tohsaka is involved, the one big thing that gets carried over (outside of her appearance) is her Tsundere nature. The exceptions are Fate/Zero, where she is noticeably less Tsundere and more of a Determinator and in a future seen in Hollow Atarxia, where she was very deredere and openly states that she can grant Shirou happiness the most, and vice versa.
Shiki here is a rather interesting case, since she doesn't fit into any one type in the dere family having parts from them all (which mirrors the concept of her powers). Is a Type Tsun, she has hints of a Yandere (whom is both Possessive and Obsessive to a degree), Kuudere (mostly by Non-Verbal Cues and is a Cynic). That said... the dere is all the same, directed specifically at Mikiya Kokutou and no one else. Shiki Ryougi can and will fight to keep this status quo with Mikiya, and god help you if you are in the way.
Also from Kara no Kyoukai is Azaka, Mikiya's sister, who is in love with him. Atypically, she acts almost entirely dere around him- Shiki is the one who gets to see both sides of her. Azaka likes and respects Shiki, but sees her as a rival for Mikiya's affections, which brings out her tsun qualities.
Sawatari Makoto from Kanon is one of the rare female examples who eventually becomes a Defrosting Ice Queen. In the last few episodes where she appears, she doesn't say one mean word. Knowing you're going to die will do that to you.
Mizuha in G-Senjou no Maou, though you might not realize it at first because of Kyousuke's limited interaction with her until you actually reach the point you can choose to start her story. She actually does a pretty decent job of making it look like she hates him in the events leading up to said point, but once you get Kyousuke close to her you'll find she's a tad spoiled with a tendency to cry when plans to admit her long standing feelings don't work out.
Shizune Hakamichi from Katawa Shoujo is a bit of a subversion. She appears to be this at first, though if you go down her path one sees that she isn't that combative in her personality to really qualify. Doesn't stop the fandom from portraying her as such however.
Angel Starr from Phoenix Wright: Ace Attorney goes from angelic to demonic and back again frequently in the course of the case she appears in.
Franziska von Karma is a young woman with an absolutely vile temper, a tendency to Whip It Good at the slightest provocation, and a fixation on perfection, but a terrific soft spot for the painfully codependent Adrian Andrews, who she eventually helps train into being able to stand on her own two feet. She finally cracks at the end of Justice For All and bursts into tears at a display of kindness from Miles Edgeworth, who she considers to be her 'little brother' even though he's older than she is. By Trials and Tribulations she's acting hostile more out of habit than anything else, and shows a soft side around children, being genuinely heartbroken when little Pearl Fey yells at her and calls her out. Phoenix even thinks to himself that her outright hostility is what makes her "cute". Granted, he also notes that he might be thinking that due to having a fever of 102.2, but that doesn't change the fact that the thought is true; that is one of Franziska's charms. Franziska also follows Phoenix for the investigation and gets pissed at Godot when he refuses to help Nick with evidence.
Ema Skye in Apollo Justice: Ace Attorney qualifies as a tsundere. She's nearly always in a foul mood, said mood gauged through her incessant munching on snackoos, and the harder she chews the more angry she is until she'll outright throw snacks at Apollo. Offer to help her do something scientific, however, and her sweet side shows up. It is ambiguous in the games as to whether Ema simply does not like Klavier or if she is tsundere for him. This is cleared up in Odoroki Gyakuten where it becomes incredibly evident that she is actually tsundere. It appears that deep down she likes him but is too afraid to admit it◊.
Gen-san is the only real tsundere in Maji De Watashi Ni Koi Shinasai, as lampshaded by others in the family. He manages to invoke I Was Just Passing Through pretty much every time he "happens" to lend a hand. The only girl on the heroine side who comes even remotely close is Chris, and even she starts dere-ing it up rather quickly. This may, however, change in the sequel, with the advent of Fushikawa's storyline.
Christiane could also be argued to be a Tsundere, but not really leaning on either side of the spectrum. There are multiple points throughout the different routes where she turns bright red from Yamato teasing her, including "SHUT UP!!" and "YOU IDIOT!" being thrown around.
Sono Hanabira has not one, not 2, but 4 Tsunderes. But the one who fits Harsh is Reo. She is about as violent as Taiga towards her lover Mai, often biting her and acting like a Jerkass, however as the game goes on, she mellows out and actually cares for Mai.
Rin from Little Busters! is a bit of a borderline example. Around the people she knows she definitely tends towards a grumpy, blunt personality, but how aggressive she is depends on who she's talking with - around Masato she won't hesitate with the high kicks, but protagonist Riki is easily able to get her to smile comfortably - and when she's around people she doesn't know she acts very shy and awkward rather than angry or sweet.
Lucia Konohana from Rewrite. She even has some special gloves for punch Kotarou.
The protagonist of Dra Koi is rather tsuntsun towards the dragon, though this is a perfectly reasonable response considering how fond she is of blowing stuff up or forcing him to do whatever she wants.
Ivan Fiore from Lucky Dog 1, who starts out as openly disdainful and mocking of Gian, progresses to huffing out a variation of "S-shut up!" whenever Gian teases him or tells him that he's smarter than he initially took him to be, and ends up admitting to Gian that being with him is all the happiness he needs. His tsundereness is best exemplified by the scene immediately following their first full-fledged sexual encounter in which he keeps on accusing Gian of how he must have attracted the sexual favors of various other acquaintances too only to clam up when Gian (correctly) retorts that he's saying all of this out of pure possessiveness.
Clover from Nine Hours, Nine Persons, Nine Doors is a non-romantic version. She's normally very friendly and sweet until someone tries her patience, then she very quickly turns rude and condescending.
Also never make fun of her brother Snake in front of her. Gods help you if you do.
Shiki Tohno of Tsukihime - an unusual example in that he's a male and the games' protagonist. In most of the routes he's a classic example of Nice Guy— cordial and well-mannered towards his love interest and just about anyone he meets - except for the closest-to-canon Arcueid route. There, he spends a large amount of time with Arcueid verbally insulting her, bringing up the fact that she's a vampire and not human, and complaining that he doesn't understand how her brain works. Arcueid being Arcueid, she doesn't mind.
Shiki: I'm basically nice to everyone. Well, recently there's been an exception to that.
Arcueid: Ahaha, that's me!
He acts like this towards his friend Arihiko as well— not in a romantic sense, despite their occasional moments of slight Ho Yay— he says that he has "loads of sympathy for anyone but him" and generally they spend most of their time together not getting along and very badly so, but they're quite obviously very close and good friends in spite of that.
Marie Miwa from Ace Attorney Investigations 2. A prison warden who makes a habbit of hugging everyone she meets, and treats the inmates as one big happy family. An animal lover who strongly believes 'animal therapy' will lead prisoners to reform. She is, however, a lot more dedicated to her job that one might think, and is pretty harsh with the guards when she finds out one of the inmates has escaped. This especially shows when Edgeworth finally confronts her at the end of the case. Unlike most other killers in the series (especially the one from the preveous case) she doesn't make much of an effort to argue back... until Edgeworth REALLY pushes her, and then she proceeds to turn his entire argument on its head with one sentence.
Fujibayashi Kyou of CLANNAD - Though she is a particularly agressive Sweet, she still favours a friendly personality over a confrontational one. She is very quick to switch to tsun-tsun mode, though.
Pick any princess from Princess Waltz. Except for Shizuka and maybe Lillian. But especially Angela and Chris.
Teru Saeki in Tokimeki Memorial Girl's Side 2 is a complicated example who vacillates between types depending on which persona he's putting forward at the moment. Initially he seems Sweet, nice to most of his classmates but rude to the protagonist; spending more time with him reveals him as more Harsh, since his rude behavior is his real self while his "school idol" persona is just a front. Eventually he softens toward the protagonist, but gets angry and runs off if things get too romantic, ultimately making him Sweet.
Though Mion's tsundere-ness is in debate, one of the TIPS from the VN pegs another Sonozaki as having the attitude of one: Oryou. Mion speculates this due to Oni-baba's decision to sell off land in an attempt to get new people to come to Hinamizawa and help erase the extreme prejudice against the Houjous, rather than work against it directly.
Satoko also presents some tsundere-like characteristics.
Jessica Ushiromiya plays it in a similar way as Mion. Shannon even lampshades it in the game.
Shannon: I believe you are what they call a "tsundora". I think this type of personality will be very popular in a few years' time...
Eventually, Battler and Beato are tsundere for each other, as part of their ongoing Mind Game Ship. And, of course, before that there is the episode where Beato suddenly goes completely deredere to outmaneuver Battler. When she triumphantly reveals her plan, she explicitly refers to this trope.
Satan from the Stakes of Purgatory is described by her sisters as "a tsundere, but without the dere".
Back to Tsundere! I swear, the only reason you lust after 2D girls so much is that you're not man enough to handle the real thing...N-not that I'd be interested in showing you! Stop grinning like that, pervert!