She was the first African-American female photographer whose work was acquired by the Museum of Modern Art (MOMA) in New York City.

She has employed a range of surrealist techniques: photographing her subjects from oblique angles, shooting out of focus or through such atmospheric effects as fog and shadow, playing on unusual juxtapositions, even altering or painting over prints.

[7][8] Smith has photographed many important black cultural figures during her career, including Alvin Ailey and Nina Simone.

"[10] Two years later (1975), Smith became the first female member of the Harlem-based photography collective Kamoinge, under director Roy DeCarava.

[11] The Kamoinge Workshop was founded in New York in 1963 to support the work of black photographers in a field then dominated by white men.

The collective, which still exists today, has undertaken a range of initiatives, including exhibitions, lectures, workshops, and the publishing of portfolios for distribution to museums.

Shortly after, she became the first Black woman photographer to be included in the collections of the Museum of Modern Art (MOMA) in New York City.

[13] In addition to the MOMA, Smith's art has been featured at the Schomburg Center for Research in Black Culture and the Smithsonian Anacostia Museum & Center for African American History and Culture in Washington, D.C. Smith's photographs are included in the 2004 Ntozake Shange book The Sweet Breath of Life: A Poetic Narrative of the African-American Family and Life.

[18] That same year, Smith was featured in the Tate Modern group exhibition Soul of a Nation: Art in the Age of Black Power, curated by Mark Godfrey and Zoé Whitley.