White Destiny from Pretear. Morning Grace from Princess Tutu and Aiyaa Four Thousand Years were my two top, boven candidates, but since they're taken, I'll go with my current favoriete song. I mean, just listen to it! This song is the reason I adore Yoko Ishida(she sings it, btw)!<3333 Pretear is the only anime I've ever watched where I didn't start skipping the intro after the first few episodes.
Another anime song I really love is Brothers from FullMetal Alchemist. Vic Mignogna's English version is just so gorgeous, I can't even begin to explain it! It's even sadder if you've seen the anime and u know what Ed's been through... T~T
Brothers:
link White Destiny: