Born in Jacksonville, Florida, Bonds was living in Norfolk, Virginia in the 1950's when he began singing publicly in church, and with a group called The Turks. He joined record producer Frank Guida's small Legrand label and Guida changed his name to U.S. Bonds in hopes that it would be confused with a public service announcement advertising the sale of government bonds and thus get more airtime. Bonds' first hit was the song "New Orleans", followed up by his only Number One hit, "Quarter To Three" in June 1961. Other hits include "School Is Out", "Dear Lady Twist" and "Twist, Twist Senora" in the early 1960s. In a 1963 tour of Europe, he headlined above The Beatles. In the late 1960s, the singer came to be known as Gary U.S. Bonds.

"Quarter To Three" appears on The Rock and Roll Hall of Fame's 500 Songs that Shaped Rock and Roll list.

In the early 1980s, Bonds had a career resurgence, working off collaborations with Bruce Springsteen, Steven Van Zandt, and the E Street Band. Later hits included "This Little Girl", "Jolé Blonde", and the liberal "Out Of Work". Bonds continues to release albums sporadically, and today is a mainstay of the nostalgia concert circuit.

While Gary U.S. Bonds is mostly known for achievements within Rhythm and Blues and Rock 'n' roll, he often transcends these genres, e.g. he has been nominated for the Country Music Association's "Songwriter of the Year" distinction. He is also a honoree of the Rhythm & Blues Foundation. Bonds is an accomplished golfer and often plays celebrity PGA events.