Moore started his long association with the Western genre in films like "Outlaws of Pine Ridge" (1942), "Along the Oregon Trail" (1947), "Adventures of Frank and Jesse James" (1948) and "The Cowboy and the Indians" (1949, with Gene Autry and future co-star Jay Silverheels). He also made several penny-dreadful serials, including "The Perils of Nyoka" (1942), "Cyclotrode X" (1946), "G-Men Never Forget" (1947) and the memorable "Radar Men from the Moon" (1952).
Stardom finally came with the ABC series "The Lone Ranger" (1949-57), co-starring Silverheels as Tonto. Riding the crest of the Western TV craze of the 1950s, Moore became the idol of a generation of American youth. He missed only the 1952-53 season, when he struck for more money and was briefly replaced by John Hart. Moore spent his vacations making films: amazingly, he released eight films and two serials in 1952 alone. Among his later titles were "Desert Passage" (1952), "Kansas Pacific" (1953), "The Lone Ranger" (1956) and his last, "The Lone Ranger and the Lost City of Gold" (1958).
Moore continued playing The Lone Ranger in commercials and promotional tours (mostly for Dodge), hitting the headlines again in 1979 when Lone Ranger Television Inc. and the Wrather Corporation barred him from appearing as the character. He was forced to abandon his mask for large sunglasses until winning the case on appeal in 1985.