Merrill Moore entered Vanderbilt University in 1920. He joined the Fugitive group in 1922, while still an undergraduate, and contributed prolifically to its magazine during its four years of publication. Moore spent the summer of 1923 in Germany, and in 1924, upon graduation from college, he entered Vanderbilt Medical School, completing his M.D. in 1928.

After a year-long internship in Nashville, Moore was appointed in 1929 as neurological house officer at the Boston City Hospital. He lived most of the rest of his life in Boston, except for a period of military service during World War II. Moore studied psychiatry with Dr. William Herman (1931) and Dr. Hanns Sach (1934-1938). He was awarded a Commonwealth Research Fellowship at Harvard Medical School, where he began teaching in 1950. Moore also maintained a private psychiatric practice in Boston.

Moore successfully combined a professional career as a psychiatrist with an energetic amateur career as a poet. He composed over 50,000 sonnets over the course of his life. Moore passed away in 1957.