I love, love, love the Silent Hill soundtracks. The first game had a ton of spooky noise, sure, but after that all of the tracks had a bit of melody to them, despite being spooky as hell. The guitar and vocal tracks are really great too.

I also really love Xenosaga, particularly for the chanting tracks (Zarathustra, The Miracle, etc...), and Chrono Cross had some good ones too.

And Arcanum.