Try Serial Experiments Lain, anything by Satoshi Kon (proof that God doesn't exist: Satoshi Kon died at age 46), and Naoki Urasawa's Monster for a cross-section of cerebral anime. I don't watch anime as often as I used to, but what I do watch is either comedy of some variety or seinen. Protip: if it has an English or instrumental song as its opening, it's probably more intellectual than the typical fare.
Since I like summarising animes through AMVs, here's a selection:
Monster - Terrifyingly realistic, set in 1990s Eastern Europe just after the collapse of the Berlin Wall.
Serial Experiments Lain - Philosophical cyberpunk, pondering the future of the internet and identity.
Paprika (Satoshi Kon) - Psychological thriller, totally warped but incredible.



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