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)