Ames attended Philips Academy, Andover, Massachusetts, then went to Harvard College, where he earned a law degree, and where his most influential teachers were George Santayana and William James (whose daughter he was also engaged to, but did not marry). After practicing law for a few years, Ames abandoned it to become a painter. For several years, while collaborating with his sister, Blanche Ames (who was also a painter), the two of them tried to determine if the quality of visual art could be improved by the scientific study of vision. Ames set about improving his knowledge of the optical components of the eye, assuming that once he had mastered them, he would return to painting. As it was, his studies mastered him and Ames made vision his life's work.