As a student at the Slade School of Fine Art, Carrington met fellow artists including Paul Nash and Mark Gertler. On leaving the Slade in 1914, she fell in with members of the Bloomsbury Circle and Virginia and Leonard Woolf commissioned a series of woodcuts from her. She also featured in Aldous Huxley's first novel Chrome Yellow (1921).
Carrington formed an especially close attachment to another Bloomsbury member, the writer Lytton Strachey (1880–1932), despite Strachey's homosexuality. The pair set up house at Pangbourne, Berkshire, and their relationship developed regardless of Carrington's marriage in 1921.
Carrington's artwork includes striking portraits of Strachey and other literary associates, including E.M. Forster. Following Strachey's death in 1931, Carrington committed suicide in March of the following year. Largely overlooked in the mid-20th century, her artwork gained a new audience in the 1990s. Her life was the subject of a film Carrington (1995) with Emma Thompson in the lead role.