At thirteen, Charles Calverley was bound for seven years as an apprentice to an Albany stonecutter. Near the end of that period, the local sculptor Erastus Dow Palmer paid for Calverley's release and employed him in his own studio. The aspiring sculptor worked there from 1853 to 1868, helping Palmer finish such works as his famous White Captive, for which Calverley did the casting and some of the actual carving on the final marble version (1859, Metropolitan Museum of Art, New York). Through Palmer, he met the artists George H. Boughton, Charles Loring Elliott, James M. Hart, Homer D. Martin, and Launt Thompson, among others. In his spare time Calverley explored his own creative energies by modeling medallion portraits of friends and members of his family. The first of these was of his mother.
In the autumn of 1868, Calverley moved to New York and opened his own studio. He soon became known for his portraits, especially his medallions in which Palmer's influence is clear. Only rarely did he execute full-length statues. Among these are his Robert Burns in Washington Park, Albany (unveiled 1891) and the allegorical Meditation (1902) in Albany Rural Cemetery.
Calverley served on the Council from 1877 to 1882. He exhibited busts and medallions at the Academy throughout the 1870s and in the early 1900s; at the Brooklyn Art Association during the early 1870s; at the Centennial Exposition in Philadelphia in 1876; and at the National Sculpture Society in 1895. Among his patrons was the New York art collector Samuel P. Avery, of whose wife Calverley executed a portrait medallion.
In his last years Calverley lived with a daughter in Essex Falls, New Jersey.