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From what I understand, Brotherhood is a lot more faithful to the manga, and also completes the story, which the first anime couldn't because the manga wasn't done yet. It has great pacing, too, building up from just the two brothers' story and some semi-random adventures to a really epic storyline that ties everything together. From what little I've seen of the original, the animation in Brotherhood is better, too. When the last season was airing in Japan a year or two ago, Hulu had the whole series subbed, with the new episodes coming in two weeks behind the Japanese broadcast (obviously this was pre-Hulu-Plus).
Oh, another series I picked up on Hulu was Trigun--a little more goofy, but also pretty sweet.
Anyway, I'll check out MPD Psycho.
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