After going on to Harvard College and graduating in 1844, he studied mathematics and astronomy under C. F. Gauss at Göttingen, Germany, during which time he published approximately 20 papers on the observation and motion of comets and asteroids.

[2] He developed and organized the service, was one of the first to determine longitudes by telegraphic means, and employed the Atlantic cable in 1866 to establish accurate longitude-relations between Europe and America.

From 1855 to 1859 he acted as director of the Dudley Observatory at Albany, New York, and in 1859 published a discussion of the places and proper motions of circumpolar stars to be used as standards by the United States Coast Survey.

Appointed in 1862 actuary to the United States Sanitary Commission, he issued in 1869 an important volume of Investigations in the Military and Anthropological Statistics of American Soldiers.

Gould's measurements of L. M. Rutherfurd's photographs of the Pleiades in 1866 entitle him to rank as a pioneer in the use of the camera as an instrument of precision; and he secured at Córdoba 1400 negatives of southern star clusters, the reduction of which occupied the closing years of his life.

The atlas introduced the system of defining constellation boundaries along lines of right ascension and declination, which was officially adopted by the International Astronomical Union for the whole sky in 1930.

[6] The catalog assigned Gould designations to all bright stars within 100 degrees of the south celestial pole in a manner similar to what Flamsteed had earlier done for the northern hemisphere.