"Akira" and "Nausicaa of the Valley of Wind." Both are based on manga, and the original stories go FAR beyond the scope of the anime. They are still classics, though. Nausicaa is one of Hayao Miyazaki's early films.
Oh gosh, where do I start? -Noragami -Ghost Hunt -Xxxholic -hell girl -School-LIVE -Dangan ronpa -Kimi ni todoke -Your lie in April -Kanon -Ouran High School Host Club (for when I need to laugh) And my list includes more but I'm going to stop my list here.
Oh god that is a seriously hard question. I guess the ones I loved the most are
Noragami Spice and wolf Full Metal alchemist:brotherhood xxxholic Tokyo ghoul Shingeki no kyojin Ookami Shoujo to Kuro Ouji Soredemo Sekai wa Utsukushii seto no hanayome Pandora Hearts Phantom: Requiem for the Phantom Darker than Black: Kuro no Keiyakusha