The tenth of twelve children, Chuck Harmon was schooled as an athlete at Dunbar Elementary by legendary Franklin Wonder Five basketball player Burl Friddle, Harmon played for the Washington High School Hatchets, who won two consecutive Indiana state basketball championships in 1941 and 1942. His brother Bill also played for the 1941 team.

On April 17, 1954, he became the first African American to play for the Cincinnati Reds’ franchise, known during the mid-1950s as the Redlegs. Pinch-hitting for pitcher Corky Valentine against Lew Burdette, Harmon flied out in the seventh inning of a 5-1 loss to the Milwaukee Braves at County Stadium. In that game he came to bat after another rookie, Nino Escalera, an Afro-Latin American from Puerto Rico who pinch hit immediately before Harmon to become the first black player to appear for the Cincinnati franchise.

Harmon got his first hit on April 25, 1954. Starting and leading off for the Reds at home in Crosley Field in a 3-2 win over the Chicago Cubs, Harmon singled in the first inning off Howie Pollet. He later doubled and scored on an error, and drew one walk. His final game was the site of his first, Milwaukee’s County Stadium on September 15, 1957 where, appearing as a pinch runner for the Philadelphia Phillies, he scored his final run on a double play.

In between, Harmon played winter ball in Puerto Rico with the Leones de Ponce and Criollos de Caguas clubs in the 1953–54 and 1955-56 seasons, respectively, while appearing with the Puerto Rican champion Caguas in the 1956 Caribbean Series.

In 1977, Harmon was inducted as part of the inaugural class of the University of Toledo Athletic Hall of Fame. He was inducted into the Indiana Baseball Hall of Fame in 1995.

In 1997, Golf Manor, Ohio (a suburb of Cincinnati) renamed one of its streets “Chuck Harmon Way” after its longtime resident. In addition, in cooperation with the Cincinnati Reds, a renovated ball field was named in his honor in the multi-use municipal Volunteer Park.

On April 20, 2004 (the 50th anniversary of Harmon’s debut as the Cincinnati Reds’ first African-American player), the Reds honored him during Chuck Harmon Recognition Night at Great American Ball Park. The pregame ceremonies included the unveiling of a special historic plaque, which now hangs near the entrance of the ballpark.

Harmon was married for 62 years to his wife, Daurel “Pearl” Harmon, who died in November 2009, two days before her 83rd birthday. They had three children.