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Since the posters so far seem stuck in more modern movies, and especially in what would be fantasy movies, I'll counter with some older, more real-world ones that come to mind:
Mrs. Danvers, in Rebecca
Madame Sebastian, in Notorious
The Baron de Varville, in Camille
Phyllis Dietrichson, in Double Indemnity
There's a distinction someone once made to me about villains you enjoy watching (Barbara Stanwyck in Double Indemnity) vs. ones that really scare you (Robert Mitchum in Night of the Hunter).
Freddie Jones as "Bytes", in "The Elephant Man" (1980).
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