In 1925 Alton wrote his first song "Bound For the Shore" at the age of 13, (co-written with his mother). It was published by Athens Music Co.
In 1933 they signed a contract with Victor Record’s budget label Bluebird and became regulars on the Grand Ole Opry variety program. Within three years, they had become the most popular act on the show.
Disagreements with Opry management led to the brothers leaving the show in 1939. While they continued to play and record music throughout the 1940s, they never achieved the same level of success they had with the Grand Ole Opry.
in 1946 they expanded from their acoustic two-piece arrangements into a full band, with bass, mandolin, steel guitar, fiddle, harmonica, and additional guitars. Some of those additional guitars were supplied by Merle Travis.
The most important backup musician on these sides was Wayne Raney, who played a "choke" style of harmonica that was heavily influenced by the blues. The Delmores were also leaning increasingly towards uptempo material that reflected the upsurge in Western swing and boogie-woogie.
By the end of 1947, they were also using electric guitar and drums. Raney (who also sang) in effect acted as a third member of the Delmores in the late '40s and early '50s, when they plunged full-tilt into hillbilly boogie. These are the most widely available and, in some ways, best Delmore Brothers sides. They were also the most successful, and in the late '40s the brothers reached their commercial peak, releasing a series of hard-driving boogies with thumping back beats and bluesy structures.
The Brothers recorded "Hillbilly Boogie," "Steamboat Bill Boogie," "Barnyard Boogie," "Mobile Boogie," "Freight Train Boogie," and even "Pan American Boogie." These were exciting performances featuring extended guitar solos that clearly looked forward to the rock era.
Their best-known song, "Blues Stay Away From Me," is regarded by some as the first rock and roll record. It was covered by Gene Vincent and the Blue Caps.
Rabon died of lung cancer in 1952. Alton, shaken by this loss, the loss of his father, the death of his young daughter Susan, and his own heart attack all within a three-year period, settled back in Huntsville, Alabama. He taught some guitar, did odd jobs, and devoted his creative energies to writing prose. He wrote a series of short stories, then the ambitious work of his autobiography, Truth is Stranger than Publicity, published posthumously in the 70s.
Over the course of their careers, the Delmores wrote more than one thousand songs. Some of the most popular were Brown’s Ferry Blues, Gonna Lay Down My Old Guitar and Fifteen Miles from Birmingham.
Bob Dylan was quoted in the Chicago Tribune,on November 10th 1985 as saying "The Delmore Brothers, God, I really loved them! I think they've influenced every harmony I've ever tried to sing."