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Alice was born in New Orleans of African American, Native American and Caucasian ancestry. She graduated from Straight College (now Dillard University) with an education degree in 1892.

Three years later she published her first book, Violets and Other Tales, which was a mixture of short stories, poetry, sketches, etc., which would begin a multifaceted career as an author of many genres, including fiction, drama, and newspaper journalism.

She married Paul Laurence Dunbar after a courtship of letters that began when Dunbar saw her picture accompanying one of her poems published in the Monthly Review in 1897.

They married in 1898 in a secret ceremony in New York, where she was teaching at the White Rose Mission (later, the White Rose Home for Girls in Harlem), which she helped to found. After her marriage, Dunbar-Nelson moved to Washington, D.C., with her husband.

When Dunbar-Nelson's marriage ended in 1902, she moved to Wilmington, Delaware, where she taught at Howard High School, and, during summer sessions, at the State College for Colored Students (Delaware State College) and at Howard University. Alice entered into her second marriage, with Arthur Callis, in 1910; the couple was subsequently divorced.

Her work included themes of New Orleans and Creole life, and also frankly confronted the race problem and the issues of "passing" and the "color line". A portion of her Cornell University master's thesis on Milton and Wordsworth was published in the highly respected journal Modern Language Notes in 1909.

She was widely published in journals, gave many speeches, and wrote newspaper columns for the Pittsburgh Courier and the Washington Eagle.

Her greatest contribution to the field of Black women's literature is the diary she kept in the 1920s and 30s. Being one of only two full-length diaries written by nineteenth century Black women, it addresses areas of sexuality, family, health, work, and writing; it documents the existence of an active Black lesbian network and her relationships with several prominent women. (The other diary in existence is written by Charlotte Forten).

Her activist work in race relations and suffrage included serving on the Delaware state republican committee and directing campaign activities among African American women, heading the Delaware Crusaders for the Dyer Anti- Lynching Bill, and being a member of the delegation that addressed President Warren Harding at the White House on the issue of African American concerns.

A prominent clubwoman and feminist, she was the field organizer for women's suffrage for the Middle Atlantic states.

She was a co-founder of the Industrial School for Colored Girls, in Marshallton, DE, where from 1924-28 she served as parole officer and teacher. She served as the executive secretary for the American Inter-Racial Peace Committee from 1928-1931, in which capacity she traveled widely, giving speeches and organizing programs. She died in Philadelphia, aged 60.