Coburn began taking photographs when he received a camera as a gift on his eighth birthday, but it was not until 1899, when he met the photographer Edward Steichen (Steichen, Edward), that he became a serious photographer. In the same year Coburn contributed to two important exhibitions: the New School of American Pictorial Photography exhibition and the Salon of the Linked Ring, a group of English photographers who worked to establish photography as an art.

In 1902 Coburn opened a studio in New York City to exhibit his prints, and in that same year he was elected to the newly formed Photo-Secession, a group of American photographers whose aims were similar to those of the Linked Ring. The following year he was elected a member of the Linked Ring. After working for a year in the New York studio of Gertrude Käsebier (Käsebier, Gertrude), a leading Photo-Secessionist, Coburn returned to Boston, where his style was influenced by his discovery of the ink paintings of the Japanese master Sesshū.

In 1904 Coburn left for London with a commission to photograph celebrities. Among the memorable portraits he made there were those of the writers George Meredith (1904) and Henry James (1906) and the sculptor Auguste Rodin (1906). He even made a nude portrait of George Bernard Shaw (Shaw, George Bernard) (1906) posed as Rodin's well-known sculpture The Thinker. Coburn's portraits were collected and published in the books Men of Mark (1913) and More Men of Mark (1922).

In 1913 Coburn exhibited five photographs collectively titled New York from Its Pinnacles, showing street scenes viewed from above. These photographs, especially The Octopus, New York, display a novel use of perspective and an emphasis upon abstract pattern. In 1917 he began taking the first completely nonobjective photographs. He called them vortographs to associate them with the Vorticists, a group of English writers and painters who had been influenced by Cubism and Futurism, as Coburn himself had been. Vortographs were a deliberate attempt to prove that photographers could fracture space into abstract compositions as Cubist painters and sculptors had done.

During the 1920s Coburn, who had by this time moved to England, became increasingly interested in mysticism, and he abandoned the camera in favour of spiritual pursuits. In the 1950s, however, he resumed photography and produced a number of mysteriously ambiguous photographs, such as Tree Interior (1957) and Reflections (1962). His autobiography, Alvin Langdon Coburn, Photographer (1966), was edited by Helmut Gernsheim and Alison Gernsheim.