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For anime soundtrack I would say ghost in the shell.
I'm really fond of the Fullmetal Alchemist score, particularly the "Brotherhood" theme. I enjoyed a few of the songs from the opening/ending credits, though not all. Last I'd checked, the US releases only cover a fraction of what the Japanese CDs do, which is a shame. (And I'm too cheap for imports...)Naruto's "Konoha" theme is quite nice as well, as are a few of the opening and closing songs.I enjoyed the .hack//Roots score. It's got some interesting variations on themes from classical music, plus plenty of original music. I happened upon the CD at GimmeAnime's booth I think at the last NDK (maybe it was Starfest?) and had to buy it. I'm glad I did.Evangelion's got some good music, and I've got I think all but one or two of the various CDs they've released... which means I own about 12 copies of "Fly Me to the Moon." Haibane Renmei's score is one of my favorite anime scores, and I picked up the soundtrack immediately after watching the show. Unfortunately, they domestic CD doesn't have the "Blue Flow" song from the end credits, likely for licensing reasons. (Naturally, if I bought the import instead, it'd be on there. *sigh*)Millennium Actress had some fantastic music as well, though I've had trouble locating a soundtrack for it. I guess it wasn't popular enough in the US to get a release.And, of course, one can't forget the music of Joe Hisaishi from Miyazaki's films. I particularly enjoyed the Princess Mononoke and Spirited Away scores.As for the "best?" I couldn't say. I've not heard them all, and I don't think I could pick out the "best" even if I had. I've got a few that I enjoy more than the others (notably FMA, Haibane Renmei, and Spirited Away), but I'd have trouble even picking out a favorite. Cop-out? Sure. But there's no one soundtrack that sticks out in my mind as the "best."
Evangelion's got some good music, and I've got I think all but one or two of the various CDs they've released... which means I own about 12 copies of "Fly Me to the Moon."
By the way greg, where did you get the world of goo soundtrack? Its probably my favorite 8bit music.
The World of Goo isn't an 8-bit soundtrack, though it does have one 8-bit track (#19: "Hello, MOM"). The rest of the tracks are more or less normal.At any rate, it does have a great soundtrack. It employs many different musical styles, so it stays interesting throughout. You can download it for free (legally!) from the composer's web site. Highly recommended!
I loved the "Einhander" sound track. Also Mega Man 2 and 3. Surprised no has mentioned the "Legend of Zelda" yet.
I loved the OST for the Initial D Series... also Like mentioned aboveBeck,Cowboy beboop,.hacks,fullmetal alchemist,FCLC,