John Kramer/Jigsaw (Saw 2004)

Commander Rourke (Atlantis: The Lost Empire)

Technically king candy/turbo is a twist villian so him

Good ol' King Andrias. I love that we were clued into him being up to something in advance, which made you suspicious, but it was kept just vague enough for there to be a room of doubt to his true intentions

Also Hugh Ransom Drysdale and Miles Bron I guess

Rose Armitage

Omni-Man scared me every time I see him interact with characters. His villainy was exposed in the first episode and seeing him continue being friends with other characters was terrifying. In just a second, he could easily betray them in the most unsuspecting manner, while you are aware of his actions.