IMO the most kick ass:
MK1

MK2

MK3

MK4

MX vs ATV Unleashed

Need for Speed Underground 2

Prince of Persia Warrior Within

Smackdown vs Raw use to have good tracks before they started playing the worst WWE superstar music(minus CM Punk)

Guitar Hero 3 (i love my rock music)

Star Wars The Force Unleashed(1 and 2)

thats all I can think of at the moment.

Oh yea and some music for MK9 my most favorite is the new version of the Armory theme.

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James Bond 007 Goldeneye for N64

Any verison of Final Fantasy IV (but the GBA version music sounds great)


And the arcade and Gameboy verison of MK1

I have a couple of classics in mind:

Ace Combat 2-
It seems like the series has been known for its epic orchestral pieces, but AC2's soundtrack has been forever engraved in my mind:

Intro Cinematic
Select Your Aircraft

Critical Depth-
Think Twisted Metal, but underwater. Made by the same developers in 1997. Amazing soundtrack:

Battle in the Pacific Rim
Battle in the Indian Ocean

Need for Speed II-
I know I've said this before, but this game has the best main menu score I've ever heard. It never fails to send chills down my spine:

Main Menu

Freelancer-
Microsoft's space sim with another great soundtrack. Plenty of mysterious, atmospheric tracks that would intensify when an enemy was near, and would reach a climax when locked in battle:

Finale
Races and Battles

Awww, I remember that one! Very cool indeed, perfectly suited for the menus.

Resident Evil 2
Resident Evil Code Veronica X
Metal Gear Solid
Final Fantasy VII / X

Marvel vs. Capcom 2: New Age of Heroes
Mortal Kombat 4
Resident Evil REmake
Silent Hill 3
Silent HIll
The Elder Scrolls II: Daggerfall
Street Fighter III: 3rd Strike
Sonic the Hedgehog

Samples of some great music:

Silent Hill

Blood Tears

Silent Hill 2

Overdose Delusion

Heaven's Night

Silent Hill 3

Never Forgive Me, Never Forget Me

A Stray Child

Clockwork Little Happiness

Silent Hill 4: The Room

Nightmarish Waltz

Resting Comfortably

Your Rain

Silent Hill: Homecoming

Scarlet

Gauntlet: Dark Legacy

The Mausoleum

The Desert Temple

Sumner's Tower


Yep. Feast your eyes on good shit. Oh and before I forget:

Diablo

Tristram

Okay, now I'm done.(For now)

Silent Hill has the best horror game soundtrack of all time. OF ALL TIME. And its not just cause it has its scary songs... its actually the use of dramatic ones that gets you!!! That tango at the end of SH1 when u get the bad ending.... it just pierces right into you!!! Who would have ever thought a tango would fit so well in a horror game (and I'm argentinean! We put tangos into everything)

Also the Metal Gear Solid saga makes VERY good use of the amarzing soundtrack it has. MGS3 has some of the best, and in MGS4 when they use all the previous ones music! That final fight on top of the sub where you basically reminisce about the previous games and u get the lifebars and the music!?!?!? FREAKING GENIUS!!!!

The Best is Yet to Come. It fit MGS perfectly. That and Calling to the Night for MGS: Portable Ops.

Brawl had EXCELLENT music