Games with good soundtracks

Alan Wake

Guild Wars<3

AI War has amazing music but I never played the game (the demo felt boring):
Midnight
Marisa

I can't figure out this forum's system, so..

*the Bioshock Trilogy - Eleanor's Lullaby

*Fable - Temple of Light

*Braid - Undercurrent & Downstream

*SW:KOTOR 1,2 - The Sith Lords

*the Mass Effect Trilogy Love Theme

Remember Me has also an interesting soundtrack. If you're looking for something monumental, try Dragon Age.

Bioshock Infinite

Silent Hill 2, 3 & 4
I really loved the Fez soundtrack although I think it's a bit of an acquired taste
Deus Ex: Invisible War (yeah, yeah I know) features the music of Kidneythieves who I adore - their vocalist Free also voiced the character of NG Resonance! (Their album Trickster is the one featured in Deus Ex)
Tony Hawk games have great soundtracks, my favourite is the one from Tony Hawk's Underground.
The Binding of Isaac has a great soundtrack too

BioShock Another one in case that didn't convince you

Super Mario RPG

Kingdom Hearts

Oh and pretty much every Zelda game.

Lord of the Rings: Battle for Middle-Earth wins this easily.

Fallout 1
&
Fallout 2

Anything composed by Jeremy Soule. :)

edit: Here is a youtube playlist with some of his work. :)

DMC, Hotline Miami, Skyrim, Saints Row: The Third

I have a playlist on my iPod of Game soundtracks that I use at work to drown out everything else. Right now it contains Mass Effect 3 (plus free DLC soundtracks for ME3), Skyrim, Witcher 2, Bastion, and Sword and Sworcery EP. I think that's been my rotation for a few months now. They never get old.

I also love Braid's soundtrack, especially when I need to relax (or fall asleep). Very soothing.

On a related note of relaxing, I've always loved the Riven and Uru soundtracks as well.

Super Castlevania IV

• The Binding of Isaac
• Sonic CD
• Sonic 2
• Ikaruga
• FTL: Faster Than Light
• To The Moon

Skyrim and Modern Warfare 2 come to mind right now.

Besides Metal Gear Solid, Shadow of the Colossus and Kingdmo Hearts that have already been said, I'll add Final Fantasy XIII-2. A game hated by many but loved by me, and it has several awesome tunes.

Brutal Legend !!!

Rayman origins. Awesome soundtrack

Devil May Cry 3 and 4. (The previous ones had great music too but they're not on PC.)
Since you mentioned Serious Sam, I'll just say- the rest of the series. :D

As for something not mentioned yet... I'd say Borderlands 2 has really nice music too, even after 300 hours it hasn't gotten too repetitive. ^_^

Oh, yeah, some other stuff I (nearly) forgot:
Giana Sisters: Twisted Dreams.
Intrusion 2.
Super Meat Boy.

CoughCough Nier CoughCough Honestly though, I feel Nier is probably the best single player game right now. It may be a tad bit dated and only available on consoles, but it is 100% worth it. Get and play the game now. Here are some of my favorite ones:

The Wretched Automatons
The Dark Colossus Destroys All
Grandma
Ashes of Dreams

The last one actually has 4 different versions for each ending of the game. Some may be simple, but if your playing the game, the music alone is enough to give you chills.

generally most indie games; mirrors edge has a pretty good too

I really like it when a game has a memorable main theme as opposed to the entirety. So I liked games like Skyrim, To The Moon, Bastion since their themes stayed in my head long after completing the game.

Anarchy Online

I find most of what Anderas Waldetoft's work to be pretty good.
Hearts of Iron 2
Crusader Kings 2
Europa Universalis: Rome

Legend of Zelda: Ocarina of Time, Sonic The Hedgehog series (first games), Deus Ex: HR, Metal Gear Solid 2 and 3, FlatOut 2, No One Lives Forever (especially second one), Unreal Tournament, Jazz Jackrabbit 2, Guilty Gear and more...

Thomas Was Alone and Trine 2 have amazing soundtracks.