In no particular order:

Top 5 Anime

Legend of the 4 Kings
Hunter X Hunter
Berserk
Rurouni Kenshin 1st OVA
Hajime No Ippo

Top 5 Anime Movies

Grave of the Fireflies
Ninja Scroll
Street Fighter 2 Animated Movie
Fist of the North Star
Vampire Hunter D Bloodlust

Honourable Mentions:

Monster, Full Metal Alchemist, Gungrave, Cowboy Bebop, Bleach, Rurouni Kenshin Series, Akira