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

Lou Wagner

Van Snowden

Hommy Stewart

Pat Lytell

Buddy Douglas

Jon Linton

Bob Howland

Scutter McKay

Roberta Keith

Penny Krompier

Brooks Hunnicutt

Barrie Duffus

Evelyn Dutton

Tony Barro

Ken Creel

Fred Curt

Dennis Edenfield