At the risk of sounding like a huger nerd, I will say that Evangelion's good, but I like RahXephon a lot more. The Eva kids are just a hair too angsty for me. Can't go wrong either way, though.
The best animated series ever is Now And Then, Here And There. The animation isn't too charming, but get past that and you'll find a masterpiece.
Rocko's Modern Life was awesome too.
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It's grime time.