There's no way to pick a single favorite for an avid anime fan. Ralnab has already mentioned Kara no Kyoukai so:
- Sen to Chihiro no Kamikakushi (Spirited Away) and Mononoke Hime (Princess Mononoke) mostly because of childhood nostalgia. Studio Ghibli's gems either way.
- Steins;Gate Fuka Ryouiki no Deja vu because it gives a very good closure to an overall great (in all aspects) series.
- Psycho Pass movie because that series had one of the most intriguing futuristic, well-paced plots I've ever come across.
- Code GEASS Akito the Exile movies, since the original title is ranking in my top five of all genres. Top-notch mecha animation and combat, intelligent plot.
- Hellsing Ultimate(5 movies) for its bloody uniqueness (literally) and.. Arucard OPness! Not for the faint hearted.
There are tons more of great movies but listing more would probably discourage the OP.
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