The Joker
Heath Ledger's joker didn't involve any CGI, but those scars on his face are thanks to special effects makeup. The face paint was purposefully messy in order to add to the chaotic nature of the role. With several iterations of the character gracing screens after Ledger, none have managed to capture the pure evil of the role like he did.
Jigsaw
The Saw franchise's main villain, Jigsaw, was portrayed by Tobin Bell, and that elaborate costume was exactly that, a costume. No CGI was involved in this villain's creation, which makes it even creepier. No one can ever forget his iconic line: "Want to play a game?"
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