Definately the original Alone in the Dark soundtrack (first played AitD when I was about 10, scared the shit outta me.)
Would add to the CnC love-in, I regularly listen to the CnC1+RA1 soundtracks.
FF7 is a fave of mine, got some great remixes.
Absolutely love the Ultima music, especially from U6, U7 and Underworld 1+2.
Elite 1-3 introduced me to some classical tracks
Daggerfall has a great score
Doom is fantastic
Quake II is bloody brilliant
Of course the Monkey Island series is super.
And you can't forget the magic of Sierra games music.
All told, I think I have almost 2gigs of game music... as if I wasn't a big enough geek eh?
Some good sites for you're perusal...
[url=http://soundtracks.mixnmojo.com/]Lucasarts [url=http://www.youtube.com/watch?v=4nigRT2KmCE]Something special...