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That opening scene of Inglorious Basterds is an absolute brilliant piece of filmmaking.
The way he goes from a nice guy sitting down for a cosy chat, to an ice-cold murder machine is amazing.
Darth Vader
The Sheriff of Nottingham from Robin Hood Prince of Thieves ("Cut his heart out with a spoon" - oh good old Alan Rickman)
Hans Gruber
Francisco Scaramanga
Walter Donovan (Indiana Jones and the Last Crusade).
I love Quint as a character, but once again I don't really see him as a villain.
He was trying to do the right thing and catch the shark, but his obsession just took over him and he went crazy.
I'm not seeing anything heroic in committing murder to steal drugs and money. Regardless of the motivation or circumstance. I'd say Quint & Omar are such endearing villains we can't see them as such.
I'm shocked no one has mentioned Max Cady from Cape Fear, Robert Mitchum was pretty badass in the original but De Niro took it to a whole new level in the newer version.