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Despicable is way more memorable.
I'm surprised there haven't been more comments on this one. Contrary to popular opinion, I thought these were pretty close to each other in quality, and that Despicable Me was a trifle overrated. In fact, I'm going with Megamind here (at least for now), because I found Ferrell a more memorable voice actor than Carrell (as much as I generally prefer the latter's work) and because the theme song of Despicable Me was so dang annoying.