The Smithsonian Institution engaged Yount's services to collect specimens of animals for taxidermy display in the early 1870s. Because he was successful in this first assignment, Spencer F. Baird of the Smithsonian again retained Yount's services in 1875 to collect specimens of many species of Rocky Mountain mammals. It is likely that many of these were displayed at the Centennial Exposition in Philadelphia in 1876, as extant photos of the exhibit halls show similar specimens. During those years, Yount also began his long career as prospector, achieving some success.