The Sky Crawlers - Main Theme: [link] Zan Sayonara Zetsubou-Sensei - Main Theme: [link] Pandora Hearts - Will: [link] Toradora! - Lost My Pieces: [link] NieR - Song of the Ancients (Popola or Fate version) too lazy for link Okami - Reset: Thank You Version: [link] Sword and Sworcery - Lone Star: [link] Silent Hill 2 - Theme of Laura: [link] Princess Mononoke - The Legend of Ashitaka: [link]
+anything from Kingdom Hearts +the movie Paprika also has a very interesting soundtrack ...just to name a few
Kimi Ga Inai Mirai(all 26 episodes of the Final Act woot woot, no need to mess with perfection) [link] Due note the band disbanded, reformed, and had to replace one member, yet they come out with this, arguably their best song yet(also it acts as a we're back statement in more ways then one).
As for char theme, and mood music, no one can touch Kaoru Wada, he's the John William of the anime scene, well actually better then John William, since Wada does both, where John Williams almost strictly does theme music only.
He did all the char theme, and mood music for Inuyasha(Do As Infinity, and Kaoru Wada covering 98% of the music in the series........omg well all this great music in a single anime is unheard of, what a magical combo they make(he also did music for the Record of Lodoss War anime, and other famous series as well, not to mention some video games too)
Kimi o Nosete(Ending theme to Laputa Castle in the Sky) [link]
Kiseki no Umi(Record of Lodoss War: Chronicles of the Heroic Knight opening) [link]
For games, pretty much everything Nobuo Uematsu did
Legend of Dragoon has a great soundtrack in general, but Dart's theme takes the cake [link] (It's so great it rivals that of Hanyou, Inuyasha's theme song [link] , It's that great)
Yoko Kanno. Dear GOD Yoko Kanno can make some amazing stuff. She did all the compositions for Cowboy Bebop (working alongside The Seatbelts) and Ghost in the Shell (working alongside, well, quite a few different artists). Here are some of my favorites:
The Seatbelts (Cowboy Bebop) - Space Lion - [link] Ilaria Graziano (Ghost in the Shell) - I Do - [link] Ghost in the Shell - Some Other Time - [link] Steve Conte (Ghost in the Shell) - Living Inside the Shell - [link]
the Xenogears soundtrack (Playstation) the Crono Cross soundtrack(SNES) the Jet Grind Radio soundtrack(Sega Dreamcast) a few tunes from Killer Instinct (SNES) and a few tunes from Metal Gear Solid (Playstation)
-The Touhou Project series has some excellent music, especially for the games being made by only one person. There are over 13 games spanning 16 years (making it about a year older than Pokemon), each with several unique tracks, but here are some of my favorites: [link][link][link][link][link][link][link] Plus, the series has an amazingly prolific fanbase, and the amount of professional-quality fan remixes is absolutely staggering.
-The Persona series has some great tracks, as long as you don't mind the occasional J-pop vocal (which judging by your also asking for anime tracks I'm assuming you don't). All but one song with vocals in Persona 4 are actually in English (surprisingly good English too, barring speed and accent). [link][link][link][link][link] There was also an anime made of Persona 4, which had some good tracks: [link][link]