Almost all Deus Ex soundtrack, and maybe the Synapse level was the best of them.
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Total Annihilation
Im a sucker for the witcher 1& 2. Also stardew valley/minecraft are both worth mentioning
So many great answers already, but one I don't think I've seen mentioned yet is the soundtrack for Bastion
It's nice to see so many different awnsers, gaming has just so many good soundtracks.
Personally, I love the soundtrack of the original Xenoblade Chronicles. "Engage the Enemy" really hits during the cutscene it plays.
Another recomendation is Xenoblade Chronicles 3's "Words that never reached you"
I think Zelda: Wind Waker's ost is one of the greats. I'm also surprised nobody has mentioned Earthbound and Mother 3 yet. They have amazing atmospheric tracks like nothing else.
Final fantasy 6 Chrono trigger Street fighter 2 Street fighter v Super Mario Bros 3 Mega Man 2 Undertale And this is really unfair but Def Jam fight for New York
The song from the first level of Sonic Adventure 2 (the one about escaping the city). It catchy to listen to while all of the action of Sonic unfolds.
I love soundtracks from Splatoon, all series. Especially Chip Damage/Blitz it! is my favourite.
Team Fortress 2 OST
I’ll add two of my favourites that haven’t been mentioned yet - Metroid Prime is my all time favourite and Horizon: Zero Dawn and Forbidden West which I’ve been listening to a ton late lately
Not sure about best but the music the black mesa game did for the half life remaster was amazing.
Pretty much the entire Castlevania : Symphony of the night soundtrack... It's all so good. And nostalgic too. One of my favorite games, and favorite soundtracks.
IDK if it's best of all time but the soundtrack to Guardians Crusade, a jrpg for kids on the PS1, is pretty up there and waaaaaaayyyyyy better than it has any right to be.
For me personally some of my favorites (most memorable) are:
Hitman 2: Silent Assassin main title (and first half of the OST)
Divinity Original Sin 2 main title
Original vanilla WoW main title music
Sanctuary from Borderland 3’s OST
BFG Division from DOOM
Pretty much the entire Skyrim soundtrack
Most of the Witcher 3 soundtrack. My favorite is probably On the Champs-Désolés, which is from the Blood and Wine expansion.
90% of the Sonic Frontiers "Cyberspace" tracks are S tier. The best soundtrack in recent memory.
There is a reason Touhou has two fandoms, one for its games and the other for its music. The music alone saved it from being another Oregon Trail and eventually got it its own anime.
Others have mentioned kingdom hearts, donkey Kong country and Jet Set Radio Future which are some of my favorites, but another one I love is Maplestory. Great simplistic map BGMs that I still listen to quite often when studying or focusing
And now I've got the Henesys music playing in my head. Old MS was so fun back in the day. Mesos pls :'(
Some great ones:
Gyruss (arcade)
Bubble Bobble (arcade)
WipeOut 2097(XL) (psx - probably the best example of songs that compliment the gameplay)
Afterburner II (arcade - just one specific track called City 202, at time 15:34)
Edit: 2 more
720 ( arcade - blistering)
Rolling Thunder ( arcade - max funky )
Def hollow knight, I think it captures the essence of a long decaying kingdom perfectly.
Personally, Quake (1996). I remember playing it as a teen and actually feeling my heart rate increase with the music. It was the first game that the music really immersed me into the game.
Honorable mention, The Housebuilding Song from RDR2. Just a perfect way to lighten the mood after such a hard hitting chapter.
Right now I'm going to have to go with a tie between Brok and Graff from Brok the Investigator and the legacy soundtrack piece After The Flames by Josh Woodward from SuperTuxKart.