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I usually play multiplayer games, so I can't judge too many games' soundtracks, but usually they were good enough for me. :) Lord of the Rings Online and L4D have awesome music, so no need to have MP3s playing in the background. When I play competitive titles, like TF2 or CoD4, I prefer to keep to the in-game sounds, as it's important to hear what's going on around you and keep track of your surroundings. :)
At the moment I'm finding it very fun to listen to classical music while playing TF2 and Zombie Panic: Source. It's such an odd and entertaining juxtaposition.
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Sven: I remember having had a Prodigy EP (Smack My Bitch Up) in my computer CD player the first time I tried GTA 1 demo.
The first time I "borrowed" a car, the CD started on its own and it was just... awesome. The perfect soundtrack !
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That EP is so good man. No Man Army is sooo gooooood. Tom Morello + The Prodigy? Oh god yes. :)
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Cameron: What music do you all listen to while gaming?
Personally, I listen to a lot of MF Doom while I play Fallout, I think it fits pretty well with the atmosphere of the game

I usually don't listen to anything, but sometimes I really enjoy listening to mashups aplusd is probably my favorite mashup artist right now.