I love the villains that can pull off narcissism just right. If you've played Tales of the Abyss, they kind of poke fun at the stereotypical full-of-himself villain type with Dist. He's convinced that he's the most beautiful being on earth, but nobody takes him seriously as he is constantly teased.
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Oh, another antagonist that I love is a huge spoiler, so read at your own risk. From Persona 4... If you plan on playing this game and don't want it ruined, don't read!
Spoiler: Adachi! I wasn't even entirely fond of this guy after I beat the game, but after I went over everything he said and did while in the TV, I came to really appreciate what a hilarious villain he is. I actually suspected him in the beginning of the game as the murderer, but then not so much towards the middle of the game. I'm not sure what threw me off, I think I just forgot about Adachi for a while.
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