Cast
- Bob Keeshan as Captain Kangaroo and The Town Clown
- Hugh "Lumpy" Brannum as Mr. Green Jeans, the New Old Folk Singer, Percy, Uncle Backwards, Mr. McGregor, and Mr. Bainter the Painter
- Cosmo Allegretti as Bunny Rabbit and Mr. Moose (both of which he also created), Dennis the Apprentice, Miss Frog, Mr. Whispers, Dancing Bear, Grandfather Clock, Uncle Ralph, was the voice of Aniforms puppet TV Fred (a live-action on-screen puppet that appeared behind the blackboard in the Treasure House), and was the artist behind the Magic Drawing Board.
- Sam Levine as the The Banana Man; the character was created by Adolph Proper (1886–1950).
- Bill Cosby as himself, the host of the Picture Pages segment (1980–1984)
- Debbie Weems as Debbie (1973–1977) and provided the voice for the puppet character Baby Duck
- James Wall as Mr. Baxter (1968–1978)
- Carolyn Mignini as Kathy and other female roles (1981–1993)
- Kevin Clash as the puppet character Artie (1980–1984) and as himself and acted in many of the sketches
- John Burstein as Slim Goodbody (1976–1980)
- Bill McCutcheon as Mr. Homan (1965–1966)
- Dr. Joyce Brothers as herself for three seasons
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