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Ergo Proxy if you're up for the mindrape and shitload of references.
Toward the Terra. Both TV and the movie is a must watch. The manga too if you aren't easily put off by the art style.
Trigun. Just so that you can read Trigun Maximum, which is godly.
Nanoha and Nanoha A's. More like a cult classic, really. Nanoha's struggle is something not present in most Mahou Shoujo.
The Melancholy of Suzumiya Haruhi. Another cult thing. Offers a different perspective that being surrounded by humanoid life form, a psychic, a time-traveler, and god of a sort isn't always fun.
Black Lagoon. Revy. Need I say more?
Blood+. How do I loved Saya?
Blue Drop. Not just the anime. The two manga are also a must. I love it for the lady-loving aliens and amusement.
Maria-sama ga Miteru. Yumi is moe and I want to be like Sei when I grow up. Need I say more?
Gundam 0079. Cult classic.
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