Lucille Bliss as Smurfette (voice)

Charlie Adler as Natural 'Nat' Smurfling / Thief (voice)

William Callaway as Clumsy Smurf / Rich Man (voice)

Hamilton Camp as Greedy Smurf (voice)

Julie McWhirter as Baby Smurf / Sassette Smurfling (voice)

Jeff Doucette as Sheriff (voice)

Bernard Erhard as Timber Smurf (voice)

June Foray as Jokey Smurf (voice)

Justin Gocke as Hans (voice)

Danny Goldman as Brainy Smurf (voice)

Kip King as Tailor Smurf (voice)

Don Messick as Papa Smurf / Chitter (voice)

Pat Musick as Snappy Smurfling / Anna (voice)

Noelle North as Slouchy Smurfling (voice)

Alan Oppenheimer as Vanity Smurf / Doctor (voice)

William Schallert as Willem (voice)

Les Tremayne as Gustav (voice)

Peggy Webber as Elise (voice)

Frank Welker as Hefty Smurf / Poet Smurf / Wild Smurf / Puppy / Rat (voice)

Jonathan Winters as Grandpa Smurf (voice)