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If we are talking just series ...
Ghost In The Shell S.A.C is the best 'thinking mans' anime.
Wolf's Rain was great on story and atmosphere.
Serial Experiments: Lain was awesomely eerie and underrated.
Evangelion is like the quintessential epic.
Many anime now are more style than substance though.
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But my person fav is rather cliche, but will always be Cowboy Bebop!! The epitome of understated cool. All the right elements. It demands respect. It is the series to expose to anyone whose ultimate concept of anime is Pokemon.
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