Bruce Reitherman provided the voice of Mowgli, who is the main character of the film. Mowgli is an orphaned boy, commonly referred to as ''man-cub'' by the other characters.
Phil Harris voiced Baloo, a sloth bear who leads a carefree life and believes in letting the good things in life come by themselves.
Sebastian Cabot voiced Bagheera, a serious black panther who is determined to take Mowgli back to the village and disapproves of Baloo's carefree approach to life.
Louis Prima voiced King Louie. King Louie is an ape who wants to be a human, and offers to let Mowgli stay in the jungle (by bribing him with bananas) if Mowgli shows him the secret of ''Man's Red Flower'' (fire), though why he wants it is unknown.
George Sanders voiced Shere Khan the tiger, who wants to kill Mowgli. For this reason the Wolf Council votes to send Mowgli away.
Sterling Holloway voiced Kaa the python. Kaa is determined to catch and eat Mowgli before Shere Khan does.
J. Pat O'Malley - Colonel Hathi the elephant / Buzzie the Vulture
Verna Felton voiced Winifred, Colonel Hathi's wife. It was Felton's last film role, with her dying one day before the death of Walt Disney, during the film's production.
Clint Howard voiced Junior, Colonel Hathi's son.
Chad Stuart - Flaps the Vulture
Lord Tim Hudson - Dizzie the Vulture
John Abbott - Akela the Wolf
Ben Wright - Father Wolf
Darleen Carr - the Human Girl
Leo De Lyon - Flunkey the Baboon
Bill Lee - Shere Khan's singing voice
Hal Smith - The Slob Elephant
Terry - Thomas - Elephants' singing voices
Digby Wolfe - Ziggy the Vulture
All of the voice actors are credited in the film's credits, with the exceptions of Leo De Lyon, Bill Lee, Hal Smith, Terry-Thomas and Digby Wolfe.