Anything Final Fantasy. Even the ones that are not *gasp* Nobuo Uematsu (heck, I don't care what haters say, FF13's soundtrack was beautiful without Uematsu). Anything Yoko Shimomura (Kingdom Hearts, Legend of Mana, etc...) Anything Shoji Meguro (Persona series). That man is just way too awesome with his music...
Hitman and Deus Ex soundtracks are great. Skyrim (TES games in general) has a great soundtrack as well as the Metal Gear games. The Mass Effect soundtracks are damn chill even though I don't like ME