Bontemps was born in the city of Alexandria, Louisiana to the son of Charlie Bontemps and Marie Pembrooke Bontemps. His birthplace at 1327 Third Street has been recently restored and converted for use as the Bontemps African American Museum. It is included on the Louisiana African American Heritage Trail.

When he was seven, his family moved to the Watts district of Los Angeles, California in the Great Migration of blacks out of the South to cities of the North, Midwest and West. He graduated from Pacific Union College in California in 1923. After graduation he went to New York to teach at Harlem Academy. In New York he became an important contributor to the Harlem Renaissance where he met many lifelong friends including Countee Cullen and Langston Hughes. Hughes became a role model, collaborator, and dear friend to Bontemps.

He began writing while a student at Pacific Union College where he majored in English and minored in history, and later became the author of many children's books. His critically most important work, The Story of the Negro (1948), received the Jane Addams Book Award and was also a Newbery Honor Book. He is probably best known for the 1931 novel God Sends Sunday, the 1936 novelBlack Thunder, and the 1966 anthology Great Slave Narratives. He also wrote the 1946 play St. Louis Woman with Countee Cullen.

In 1943, after graduating from the University of Chicago with a masters degree in library science, Bontemps was appointed librarian at Fisk University in Nashville, TN. He held that position for 22 years and developed important collections and archives of African-American literature and culture, namely the Langston Hughes Renaissance Collection. After retiring from the Fisk University in 1966, he worked at the University of Illinois (Chicago Circle) and Yale University, where he served as curator to the James Weldon Johnson Collection. Through his librarianship and bibliographic work, Bontemps has become a leading figure in establishing African-American literature as a legitimate object of study and preservation.

Bontemps died June 4, 1973, in Nashville, from a myocardial infarction (heart attack), while working on his autobiography. In 2002, scholar Molefi Kete Asante listed Arna Bontemps on his list of 100 Greatest African Americans.. Bontemps was a member of Omega Psi Phi Fraternity, Inc.

(Unless noted otherwise, Bontemps is the main author of the work)

• God Sends Sunday, (New York, Harcourt, Brace and Co., 1931)
• Popo and Fifina, Children of Haiti, by Arna Bontemps and Langston Hughes, (New York: Macmillan, 1932)
• You Can’t Pet a Possum, (New York: W. Morrow, 1934)
• Black Thunder, (New York: Macmillan, 1936)
• Sad-faced Boy, (Boston: Houghton Mifflin, 1937)
• Drums at Dusk: a Novel, (New York: Macmillan, 1939)
• Father of the Blues: an Autobiography, by W.C. Handy: edited by Arna Bontemps, (New York: Macmillan, 1957)
• Golden Slippers: an Anthology of Negro Poetry for Young Readers, compiled by Arna Bontemps, (New York: Harper & Row, 1941)
• The Fast Sooner Hound, by Arna Bontemps and Jack Conroy, (Boston: Houghton Mifflin, 1942)
• They Seek a City, (Garden City, New York: Doubleday, Doran and Co., 1945)
• We Have Tomorrow, (Boston: Houghton Mifflin, 1945)
• Slappy Hooper, the Wonderful Sign Painter, by Arna Bontemps and Jack Conroy, (Boston: Houghton Mifflin, 1946)
• Story of the Negro, (New York: Knopf, 1948)
• The Poetry of the Negro, 1746-1949: an anthology, edited by Langston Hughes and Arna Bontemps, (Garden City, NY: Doubleday, 1949)
• George Washington Carver, (Evanston, IL: Row, Peterson, 1950)
• Chariot in the Sky: a Story of the Jubilee Singers, (Philadelphia, (London: P. Breman, 1963)
• Famous Negro Athletes, (New York: Dodd, Mead, 1964)
• Great Slave Narratives, (Boston: Beacon Press, 1969)
• Hold Fast to Dreams: Poems Old and New Selected by Arna Bontemps, (Chicago: Follett, 1969)
• Mr. Kelso’s Lion, (Philadelphia: Lippincott, 1970)
• Free at Last: the Life of Frederick Douglass, (New York: Dodd, Mead, 1971)
• The Harlem Renaissance Remembered: Essays, Edited, With a Memoir, (New York: Dodd, Mead, 1972)
• Young Booker: Booker T. Washington’s Early Days, (New York, Dodd, Mead, 1972)
• The Old South: "A Summer Tragedy" and Other Stories of the Thirties, (New York: Dodd, Mead, 1973)