Posting in a "games as art" thread.
Simple answer: All games are art; it's just that most aren't particularly GOOD art. That said, I'm a bit of a connoisseur of artsy games. If you've already played the Team ICO games, Rez, and Katamari, I'd check out, in rough order:
1) Planescape: Torment. The closest thing to a Citizen Kane that the video game industry has ever produced. Simply amazing in every way conceivable.
2) Killer7 and No More Heroes, and possibly Contact. Suda51 has a reputation for developing bizarre, post-modern games, and it's a reputation well deserved.
3) Silent Hill 1-3. All three are worth playing, and all of them are disturbing in a David Lynch's Eraserhead sort of way.
4) Shin Megami Tensei: Nocturne. I can't think of very many JRPGs that are worthy of the title "artsy," since the genre is largely crap, but this one definitely is. (As a bonus, it's also one of the best JRPGs ever made.)
5) Any of the Oddworld games, but especially Abe's Odyssee and Exxodus on the PS1. Bizarre puzzle/platformers that are well worth playing.
6) Fear Effect 1 & 2. Sort of Resident Evil crossed with Blade Runner, as odd as it sounds, and one of the few games out there that would probably make a good movie.
EDIT: You may also want to watch out for Eternity's Child, a hand-drawn platformer coming to Nintendo's WiiWare service. Ever since finding out about it and seeing some screenshots, it's been up there on my "most anticipated titles of 2008" list.