Hitler from Downfall, portrayed brilliantly by Bruno Ganz. His transformation is eerie.
Cigarette Smoking Man from X-Files comes to mind (TV show I know, but he was in the X-Files movie as well). William B. Davis brought a lot of depth to a role that could have been very one-dimensional.
Dr. Strangelove
Couple more from TV: Wayne Knight as Newman, Jon Bernthal as Shane in The Walking Dead. Shredder, Krang, Bebop and Rocksteady.
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