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)