McCall was born and raised in New Jasper Township, Greene County, Ohio. He was a boyhood friend of fellow future musician Johnny Paycheck. At the age of 15, he landed a job as a disc jockey at a local Ohio radio show on Saturday mornings. During this time, he also performed as a musician at dances and other events. After graduating from high school, McCall joined the military and was stationed in Kentucky. In 1958, after finishing his duty in the army, McCall moved to Nashville with Paycheck to record as a duo. The duo failed but McCall soon found work as a background singer during recording sessions for various artists including Faron Young, George Jones and Ray Price. Next, he began to tour with the bands of Young, Price and the newcomer Hank Williams Jr.
In 1959, McCall was contacted by Nashville producer Buddy Killen, and asked to join a pop band he was forming called The Little Dippers. The band released the top ten pop hit "Forever" in 1960. The next year, McCall was signed by Capitol Records as a solo singer. He released two singles for the label, but neither charted and the performer was subsequently released by Capitol. In 1962, McCall signed with Phillips Records as a country music singer. He released the hit "A Stranger Was Here," which peaked at #17. Later in the year he performed the theme for the film Hud, which starred actor Paul Newman.
McCall decided to begin an acting career in 1965. He appeared in numerous films including Nashville Rebel, Road to Nashville and What Am I Bid. During his acting career, McCall also traveled to the American Southwest to perform in rodeos as a cowboy. In 1968, he decided to return to recording.
In 1968, McCall signed with "Wayside Records" and released four singles. In 1970, he released his first album, Meet Darrell McCall for Mercury Records. Hank Williams Jr. recorded a song penned by McCall in 1971 entitled "Eleven Roses." It became a #1 hit for Williams and resulted in a songwriting contract offer from "Tree International" for McCall, who accepted. In 1974, he signed with Atlantic Records, releasing the single "There's Still a Lot of Love in San Antone." The following year he left Atlantic and signed with Columbia records. During this period his popularity grew due to the Outlaw Country sound being pushed into the mainstream. With Columbia he recorded the hit duet "Lily Dale" with Willie Nelson, which became a top 40 hit and was awarded the "Best Duet of 1977" by Cash Box Magazine. After a few more singles with the label, McCall signed with Hillside Records in 1980 and released a single, but then decided to sign with RCA Records. With RCA, he released his final top 40 hit "Long Line of Empties." His final charting single "Memphis in May" was released for Indigo Records in 1984. In 1986, McCall recorded two albums, including one with Johnny Bush. Following these releases, he stopped recorded but continued to tour. However, he did appear as the lead singer on a few tracks of the Ace in the Hole's 1995 debut album. MFRS