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Akihiko Kayaba from Sword Art Online
Zim, Gir, and Tak from Invader Zim
The Xenomorphs and Yautjas from the Alien and Predator films are technically the villains so I'll count them
I've always liked the various forms of Buu from DBZ, but Kid Buu is my favorite
Shockwave from Transformers
Gideon Graves from Scott Pilgrim
The Lord of Owls from Usagi Yojimbo
Giegue from Earthbound
And of course: SHUMA GORATH!!!
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