For me I think it was Jack Black in King Kong. I just wasn’t prepared for Jack Black being in a more serious role.
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Kind of a cliche answer now, but at the time, everyone was shocked by Heath Ledger’s casting as Joker.
Similarly, I was initially skeptical when Robert Pattinson was announced for The Batman. But I thought he did a fantastic job!
Oh, I have a better one; Angela Lansbury in ‘The Manchurian Candidate’. As far as I know, the only time she has played a villain. And she was fantastic