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I think Christopher Lee would have been perfect if his voice hadn't already been associated with Saruman. Similarly, John Rhys-Davies's voice strikes me as quite appropriate for Smaug.
Patrick Stewart would probably be good in principle, but I'm afraid I just couldn't take Smaug seriously if he had the voice of Captain Picard.
There are some odd suggestions on that list, though. Mark Hamill? Terry Gilliam? Surely it should at least be someone with an authentic English accent (I can't imagine Smaug talking like an American).
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