I'd have to say hajime no ippo. Both seasons. Actually, I was hesitant to watch it at first cause it was boxing and I thought it would be dull, BUT NO! It's epic. Moved on to the manga after the second season ended, but word is that a third is coming sometime in October.:D
Overall best? Best story, animation, voice work, etc.? My all time favorite series is kind of odd and not very family friendly what so ever...Urotsukidoji. Who doesn't love tentacle rape and multi-penised demons?
Too many to chose from :) some of my favorites are Beck, Cowboy Bebop, FLCL, Full Metal Panic Fumoffu, Serial Experiment Lain, eveything Ghost in a Shell, Air Gear, Bleach... I could go on forever lol.
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