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Mr Khan said:
Justice League/Unlimited. It was the culmination of everything the Diniverse worked towards, and it showed. Earlier entries (including the vaunted Batman: TAS) were often rough around the edges, having occasionally poor animation or dry plots. They spared no expense on Justice League (or merely the advance in technology allowed them to do more), and the diversity of heroes made sure that the episode ideas were almost universally good, and the overarching story arcs fan-fucking-tastic

Justice League had a lot of inconsistent writing...

If Avatar counts, then Avatar.  Haven't been so emotionally invested in characters since Lost.

If not, then Batman TAS.  It was classy all the way through.