I'm not sure what my all-time favourite is, actually...probably Pokemon. Back in the day, the dub was brilliant, and it stayed pretty damn awesome right up the point that they switched voice actors...now it isn't worth talking about, though >>
Now, just for the storyline alone, it'd be Ghost in the Shell: Stand Alone Complex, because each time I watch it, I see something I missed before. The action isn't too bad, either, and Tachikomas are every kind of awesome. Plus, the central antagonists, particularly Gohda, are well thought-out and aren't just your stereotypical "OMG CONQUER THE WORLD!" kind of villains...which I hate. Unless they have a suitable evil laugh and a good hairstyle. And actually do some damage before their inevitable death.
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