LogFAQs > #893102421

I don't know if you'll particularly care for game soundtracks based on chiptunes. I mean, sometimes the soundtrack is slightly enhanced, but you're still listening to chiptunes and not real orchestrations. They're great for nostalgic value if you've actually played the games, though.

Anything from the Elder Scrolls series would be a good place to start. If you want something more brooding, then the Fallout 3 and New Vegas soundtracks (which I believe were released in digital format only) have some really nice atmosphere.