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30 Days of Marvel: Day 20: Best cartoon version of any comic
Okay: right up front. I do not like cartoons. Some cartoons are vaguely watchable, most are not. When I do watch a cartoon, it's almost certainly out of curiosity, not pleasure. I hate the exaggerated voices, the thin stories, and, often as not, the simplified art.
X-Men: The Animated Series was rather good. I particularly liked the voice of Chris Potter for Gambit. (I have my priorities.)
The Avengers: Earth's Mightiest Heroes isn't bad... I didn't run screaming. It would probably be going too far to say I liked it, but it was fun to see my familiar heroes being revised and revisited. I liked the voice of Eric Loomis as Iron Man.
My favourite? Without doubt, Spider-Man: The New Animated Series - not so new now, as it aired in 2003. I never saw it on TV, but I liked the look of the art and bought the DVD.

Neil Patrick Harris was the voice of Peter Parker, and he was good.
I liked it enough to buy the DVD, but that was a few years ago, and I haven't liked it enough to actually watch it yet.