I would say the Naruto Ultimate Ninja storm games look very much like the actual anime. A lot of other fighting games like Blazblue and Arcana Heart also look akin to anime.

Playing it, considering it is literally anime art on a 3D plane hard to argue.  Story is standard, but I actually have been pleased witht he rhythm based combat.  If you are JRPG nut like me I'd go for it.

Otherwise I would say Atelier series or Ni No Kuni or Tales do a great job cel shading to bring anime feel to polygon models.

Good point, I'd submit Blazblue there as well.

also the Naruto Ultimate Ninja Storm series looks good; UNS1 does a really good job making Kohana while UNS3 did a really good job on it's cutscenes

Another contender:

Thousand Arms

Are we talkin about graphical or actually tone while playing game?

Tales of Xillia without a doubt

I'm actually 20 hours into it; as close to an anime as any game is going to get.

BB