I really like Akira Yamaoka's music for the Silent Hill series, but I have to admit each individual game's soundtrack has at least one cheesebomb that goes too far for me (re: "as albums"). Luckily there is this:

'The Music of Red Dead Redemption 2 (Original Score)' is good, and uses a lot of Colin Stetson, whose presence on the record I'm going to pretend is due to the appropriateness of his family name.

World of Goo is great.

The music in No Man's Sky is almost uniformly terrific. There's an official soundtrack, but apparently during gameplay it's partially procedurally generated from sounds on that soundtrack. Whatever, it's great for zooming around space!

I've always been a major fan of Lee Jackson's work in Rise of the Triad (original game), though stylistically it's all over the place and may not make a good cohesive album, per se. You can tell, though, that he had done his studying on music theory and composition. His knowledge of harmony and counterpoint are miles above many of his peers.

Shin Megami Tensei IV
Castlevania : Order of Ecclesia

Probably not for most folks but I’ve listened to these as albums. As recently as yesterday. SMTIV actually came with a CD of the soundtrack, even.

I could listen to this song for hours. And do

On top of being the finest videogame, Noita has a great soundtrack.

The Unreal soundtrack is unbeatable.

It's always difficult to judge how music would work outside the game when you know it from the game, since for me this music sounds like the colours and scenery and general atmosphere of the game. Likewise these 90s synthesizer sounds are connected to a kind of childhood fascination for me; there is a kind of mood, an evocative quality, that is close to how I feel and think about computers and computer games; like they belong together.

Nonetheless while I know nothing of that game, I could easily listen to that Shin Megami tune posted earlier for all 30 minutes, and then play it again. So I think I can be confident that it works even outside of all that.

The Unreal soundtrack was put together in FastTracker 2 and stored on the cd as .xm files (technically .umx, but as I understand it this is just a typical .xm locked into a proprietary format; it is still playable like any tracker file, just not modifiable), which had the advantage of allowing high quality music in tiny files, as well as (iirc) allowing tracks to be started at and looped around any point, which makes "event music" easy to implement.

The music was composed mainly by Alexander Brandon, with contributions from Michiel van den Bos and Andrew Sega. The former two are also responsible for the superb Deus Ex soundtrack. Andrew Sega has made fantastic music under the names Psychic Monks and Necros. Brandon has released a couple of solo albums, but oddly enough they all blow.

The Unreal Tournament soundtrack, by the same crew, is even more "album worthy", but not as significant to me personally.

Uplink, a hacker simulator from 2001. Never so much as looked at the game but this sounds way dope.