The only two that comes to my mind are Wario and Donkey Kong, who was the main villian in Super Mario Land 2 and Mario and Wario. Donkey Kong is the main villian in the Donkey kong game and the Mario vs. Donkey Kong franchise, but aside from that how many villians in the Mario universe have been the main villian in more than one game in the Mario series. Fawful doesn't count he wasn't the main villian in Superstar saga. Most other villians are one time usually.
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