-Pocket Monsters. Most dub watchers probably don't know this, since 4Kids sticks in alot of their crappy, low quality junk. But the Japanese music is actually very good, and the movie music is fantastic, especially Mewtwo Strikes Back. Great fight music as well as dramatic and adventurous stuff. The music when the Pokemon are fighting and it starts to take its toll on them is very sad and moving, and really helps illustrate the message. And the music in the Satoshi death scene is just incredible.
-Spirited Away. I LOVE this score. Hisaishi Joe is da man. Such beautiful, high quality music.
-Princess Mononoke. Another Oscar-worthy score by Hisaishi-san.
-Ai Yori Aoshi. Great love-oriented music. Very touching. And I LOVE how alot of it has a very traditional Japanese sound to it. ^^
-InuYasha. Alot of great fight music, and even better music for romance and drama. Also has alot of traditional Japanese-sounding stuff. ^^
Others, like the other Miyazaki films, Fullmetal Alchemist, the Rurouni Kenshin OVAs, etc. are also excellent.