René Auberjonois

as Stranger (voice)

Michael Bell

as (voice)

Lucille Bliss

as Smurfette (voice)

William Callaway

as (voice)

Hamilton Camp

as (voice)

June Foray

as (voice)

Danny Goldman

as Brainy Smurf (voice)

David Mendenhall

as William (voice)

Don Messick

as Papa Smurf / Azrael the Cat (voice)

Alan Oppenheimer

as (voice)

Henry Polic II

as (voice)

Alexandra Stoddart

as Gwenevere (voice)

Paul Winchell

as Gargamel (voice)