Filmation approached TV's original Lone Ranger and Tonto, Clayton Moore and Jay Silverheels to reprise their characters for the animated series, but Moore felt he could not perform without a proper amount of rehearsals, even though producer Lou Scheimer assured him that he did not need to learn any lines and would be reading his script in his hand during recordings.
William Conrad agreed to voice the Lone Ranger, but since there was still a stigma attached to doing cartoon work, wanted to be billed under the pseudonym "J. Darnoc", which is his last name backwards.
The character of Tonto uses various pieces of stock animation based on and modified from those originally created for Mr. Spock in Star Trek: The Animated Series (1973). The most noticeable of these is the shot of him turning to the camera with a raised eyebrow.
Henry Darrow who voiced Zorro will later play Zorro's father Don Alejandro de la Vega in the 1990s television series Zorro.
The Lone Ranger and Tonto previously appeared in the Brady Kids with the same voice actors.