Final Fantasy VII and Final Fantasy IX have the best OSTs of the series to me, also I like a few of other games battle themes etc. FFX seemed kind of bland to me after the masterpiece that is IX and after Nobuo left the series music went down the shitter, although XIII-2 sounds not bad actually. Other great Soundtracks?
VVVVVV
Bastion
Painkiller: Black
The Last Story, yeah, I am a Nobuo Fanboy ;)
Zelda OoT(the other games are fine too, but OH GOD THE GERUDO VALLEY)
Halo has a really pleasant score.
Skyrim's Soundtrack, especially the main theme is the best part about the game.(Yeah, I prefer the heavy choir themed stuff to the classic Morrowind/Oblivion themes)
Metroid games have fine music, too.
Sorry if this is all a bit too console centric. But I expect not to be flamed since people here seem to be more mature and less painstakingly stupid.
There are a ton of other good OSTs but those are what popped into my mind.
Most of the soundtracks are bland and boring these days, I start to feel sick the moment I hear orchestrated music most of the time. The perfect run of the mill we are as cool as Hans Zimmer music. No memorable tunes and melodies anymore, back then when the technical limitations for music were horrendous they managed to produce the most interesting melodies and themes. It is a shame that music in games, or in general, doesn't get the respect and care it deserves most of the time and yet it is those games with tunes we hum during the day and melodies that connect us to the piece fiction that ultimately helps in forging brilliant experience that we will remember for years to come.