Don Messick
— Papa Smurf (Voice)
Danny Goldman
— Brainy Smurf (Voice)
Lucille Bliss
— Smurfette (Voice)
Frank Welker
— Hefty Smurf (Voice)
Michael Bell
— Handy Smurf / Grouchy Smurf (Voice)
Paul Winchell
— Gargamel (Voice)
Hamilton Camp
— Greedy Smurf (Voice)
Alan Oppenheimer
— Vanity Smurf (Voice)
June Foray
— Jokey Smurf (Voice)
William Callaway
— Clumsy Smurf (Voice)