Two years later, at Sun Records studio in Memphis, Tennessee, producer and engineer Jack Clement discovered and recorded Lewis for the Sun label while owner Sam Phillips was away on a trip to Florida. He became a session musician playing piano for Sun artists like Billy Lee Riley and Carl Perkins. As his own career came on the upswing, hits such as "Great Balls of Fire" soon followed, and would become his biggest hit. Watching and listening to Jerry Lee Lewis, Elvis Presley allegedly said that if he could play the piano like that, he'd quit singing. Lewis' early billing was Jerry Lee Lewis and his Pumping Piano.

On December 4, 1956, Presley dropped in on Phillips to pay a social visit while Perkins was in the studio cutting new tracks with Lewis backing him on piano. The three started an impromptu jam session, and Phillips left the tapes running. He later telephoned Johnny Cash and brought him in to join the others. These recordings, almost half of which were gospel songs, survived, and have been released on CD under the title Million Dollar Quartet. Tracks also include Chuck Berry's "Brown Eyed Handsome Man", Pat Boone's "Don't Forbid Me" and Presley doing an impersonation of Jackie Wilson (who was then with Billy Ward and the Dominoes) singing "Don't Be Cruel. In 1957, his piano and the pure rock and roll sound of "Whole Lotta Shakin' Goin' On" (which in 2005 was selected for permanent preservation in the National Recording Registry at the Library of Congress) propelled him to international fame.