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Paul Winchell, known for his voice acting, played the role of Gargamel in the animated series "The Smurfs." Gargamel is the primary antagonist, a wizard who relentlessly pursues the Smurfs to capture them for his evil schemes. Winchell's distinctive voice and comedic timing brought life to the character, making Gargamel one of the most memorable and iconic villains in animation history.