My picks would be...
PC: Planescape Torment, bar-none.
NES: Super Mario Bros. 3, for obvious reasons, but Kirby's Adventure comes a close second.
SNES: Zelda ALttP. A game that proved that you didn't need to be an RPG or adventure game to tell a coherent story.
N64: Ocarina of Time, obviously.
Gamecube: Killer7. A surreal mindfuck of a game.
Wii: Super Mario Galaxy. I still stand by my opinion that it's the most beautiful game this generation, and it's a pure joy to play to boot.
PS1: Oddworld: Abe's Exoddus. Just plain awesome in every way.
PS2: Lots to choose from, but ICO would be my pick.
PS3: Don't know, as I don't own one.
Xbox: Tough choice, but I'd say Call of Cthulhu: Dark Corners of the Earth.
Xbox 360: Tie between Bioshock and Rez HD.
Also, ugh @ the MGS worship. What do people see in these games, anyway?
"'Casual games' are something the 'Game Industry' invented to explain away the Wii success instead of actually listening or looking at what Nintendo did. There is no 'casual strategy' from Nintendo. 'Accessible strategy', yes, but ‘casual gamers’ is just the 'Game Industry''s polite way of saying what they feel: 'retarded gamers'."
-Sean Malstrom