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I don't know about you, but as a music lover I love that Gog.com packages soundtracks with many of its games. Some game music can be really fantastic, while other times it can be really bad. All of the Gog.com soundtracks I own are pretty good, but some rise to the level of great. Here are my favorites from my Gog collection:

1. Under a Killing Moon: I didn't like the game very much (I much preferred Mean Streets) but I thought the soundtrack to this game was really good, especially the theme from Tex's office.

2. Outcast: I haven't played much of this game yet, but the music is absolutely incredible. The production value here is amazing for a game from the 90's. Full orchestra and choir!

3. Dark Fall: The Journal - Very short, but very good soundtrack. I don't own it, but the Dark Fall II: Light's Out soundtrack is even better!

What are some of your Gog.com soundtrack Favorites?
Fallout and Planscape Torment. No doubt about it.
Outcast's is amazing. Just like the rest of the game.

I'd definitely add Total Annihilation to the list.

If we're counting the Witcher 2 as a GOG then that's one undeniably badass soundtrack there too.

Tropico's is perfect for the game. Very hard to beat.
Total Annihilation, thats realy all that need to be said. the fact that it won the guy who made it (the awesome Jeremy Soule) a years pay just adds to it. Thinking about it any soundtrack he touches turns to gold just check out his other work, IWD, Morrowind, Dungeon Siege.

But I will admit Outcast does have an amazing soundtrack too.
Well, just the games I own...

Blood - it's amazing. Dark, mystical, symphonical, something between dark ambient and Sunn O))).

Redneck Rampage - as much as I don't like the game, the music rocks. Pure psychobilly, bumpkin punk and other jolly and rockin stuff.

Messiah - harsh, aggresive and fast industrial metal by Fear Factory. In fact, you can download the game\s OST *and* album titled Messiah, which is a compilation of FF's various tracks.

The Witcher - another excellent soundtrack - symphonic, nearly new age/neofolk pieces with lot of female vocals and traditional instruments. And additional "Inspired by" album composed of pieces by Vader, Jesus Chrysler Suicide and other various artists!

Tyrian 2000 - for last, one of the best OSTs for classic 2d shoot'em up. If you just don't recognize Rock Gardens, then your life misses something.
Oh my goodness, if you haven't heard the Far Cry theme (or main menu music), it is right up there with the Halo theme, imho. It captures the essence of the emotion of the game, gorgeous environment filled with intensity of one man trying to survive the slaughter, all odds stacked against him. FAR CRY THEME on YouTube!!! Check it out!!! :D

Rayman 2 - Pretty cool stuff for a kinda goofy adventure game! (but awesome) It's too bad it isn't longer; one should just look up the Rayman 2 soundtrack (esp. the "Final Boss Battle" song; as someone said, "Epic riff") on Youtube and download it there. It's still reasonable quality and much much longer, 5+ minutes.

Duke Nukem: Manhatt. Project - I like some of the songs, like the subway music. (Although the OST didn't actually come with it, did it? Again, find and download from YT)
Guilty Gear. A little more upbeat than I typically like but some solid metal.
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tburger: Fallout and Planscape Torment. No doubt about it.
I agree completely! Mark Morgan is one of the few game composers I listen to...
All the Infinity Engine games had outstanding music. So did everything from Origin. Divine Divinity was beautiful and moody.

Gabriel Knight series had a lot of memorable themes. Zork Nemesis had some repetitive atmospheric tracks that still run through my head 15 years later.

Last Express had long stretches with no music but made great use of music where appropriate.
Tyrian :D
Ultima Underworld 2.. I've been humming it for years
Rise of the Triad. /thread
Heroes of Might & Magic IV hasn't been mentioned yet?
Of the soundtracks I HAVE, I would say Gothic II and Under a Killing Moon.
But huge nods to the Baldur's Gate & Icewind Dale series (I have them from original release so haven't got GOG versions!)
From obvious choices, all (Ho)MM soundtracks, Fallout and IE games.

From less obvious choices, Gobliins :D These tunes are impossbile to forget.