Jack Wild as Jimmy

Billie Hayes as Witchiepoo

Martha Raye as Boss Witch

Cass Elliot as Witch Hazel (as Mama Cass)

Allan Melvin as H. R. Pufnstuf / Henrich Rat / Living Island Boat / Orville Pelican / Polka-Dotted Horse / Stupid Bat / West Wind (voice) (as Al Melvin)

Walker Edmiston as Dr. Blinky / Ludicrous Lion / Seymore Spider / Various (voice)

Don Messick as Freddy the Flute / Googy Gopher / Orson Vulture (voice)

Roberto Gamonet as H.R. Pufnstuf

Billy Barty as Googy Gopher / Orville Pelican

Angelo Rossitto as Seymore Spider / Clang

Jane Dulo as Miss Flick

Sharon Baird as Shirley Pufnstuf

Felix Silla as Polkadotted Horse

Johnny Silver as Dr. Blinky / Ludicrous Lion

Jan Davis as Witch Way

Princess Livingston as Witch

Joy Campbell as Orson / Cling / Various Characters

Andy Ratoucheff as Alarm Clock

Joan Gerber as Dowager Tree / Granddaughter Clock (voice)

Allison McKay as

Lou Wagner as

Van Snowden as

Hommy Stewart as

Pat Lytell as

Buddy Douglas as

Jon Linton as

Bob Howland as

Scutter McKay as

Roberta Keith as

Penny Krompier as

Brooks Hunnicutt as

Barrie Duffus as

Evelyn Dutton as

Tony Barro as

Ken Creel as

Fred Curt as

Dennis Edenfield as