Charles Brough was born in Clinton, Mississippi. In 1894, he graduated from Mississippi College in Clinton. He earned his Ph.D. at Johns Hopkins University in 1898, and graduated from the law school at the University of Mississippi in 1902. He taught at Mississippi College, Hillman College, and the University of Arkansas. He served as a Baptist deacon.
Brough was elected Governor of Arkansas in 1916. During his administration, the state reformatory for women was founded and a girl's industrial school was opened. He signed into law a bill which allowed women to vote in primary elections. Under Brough, Arkansas became the only southern state to allow women's suffrage prior to the 19th Amendment. Brough was a liberal Democrat and publicly opposed lynching and advocated for the passage of anti-lynching laws. He was reelected as governor in 1918.
Brough was a personal friend of the Woodward family and was an early influence on prominent southern historian C. Vann Woodward.
Brough served as the director of the Public Information Bureau from 1925 to 1928 and served as president of Central Baptist College in Conway, Arkansas in 1929. He chaired the Virginia-District of Columbia Boundary Commission from 1934 to 1935. Brough was also a Civitan.
Asked how to say his name, he told The Literary Digest: "Pronounced as if it were spelled bruff." (Charles Earle Funk, What's the Name, Please?, Funk & Wagnalls, 1936.)