Smith was born and raised in the all-black community of Mound Bayou, Mississippi. He attended Tennessee Agricultural and Industrial State College (later Tennessee State University) from 1938 to 1940, but graduated from Morehouse College in Atlanta in 1942 with a double major in music and religion. He later received a Bachelor of Divinity degree (now known as a Master of Divinity degree) from Howard University School of Religion in 1945.
Smith moved to Nashville, Tennessee in 1951 where he became pastor of First Baptist Church, Capitol Hill, a post he would retain until his death in 1984. He became president of the Nashville NAACP in 1956 and founded the Nashville Christian Leadership Council (NCLC) in 1958. Through the NCLC, Smith helped to organize and support the Nashville sit-ins—a movement which would successfully end racial segregation at lunch counters in Nashville. In a 1964 interview with Robert Penn Warren for the book Who Speaks for the Negro?, Smith comments that the end to segregation was achieved through much hardship and many negotiations by the NCLC.
Smith was married to Alice Clark Smith and had four children, daughters Joy Ardelia, Adena Modesta, and Valerie Lin, and son Kelly Miller Smith Jr. He and his wife also reared a foster daughter Dorothy Jean Springfield.
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