megafat: Quake.
Some of the best atmospheric tracks in any game ever, and all done by Trent Reznor. I've put some of that music into playlists and unintentionally spooked myself before.
I agree, the Quake soundtrack is one of a kind in the way that it can feel like you somehow get posessed by it but it can also be a meditating and soothing experience, which hasn't been matched by any other soundtrack I know of yet.
My vote goes to a more lighthearted soundtrack though, which is the OST of Rayman 2.
In contrast to Super Mario 64 for example the soundtrack has a much deeper, ambient and mysterious vibe to it, which really helps to suck you into Raymans world.
Like the atmosphere of the game, the tracks range from more upbeat to haunting.
Every tune seems to pinpoint match the situation and makes you associate the music with the moments of the game in your memory.
The game is accompanied by this soundtrack dynamically, so your actions will be underlined by certain passages, which kinda gives the music an interactive feel.
The Rayman 3 soundtrack is great too, but had an often more humorous approach and went a little more into the background, because the characters where fully voiced now and were talking during gameplay too.
I still hope there's a proper Rayman 4 coming someday!