Edwin Cortlandt Bolles was born on September 19, 1836, in Hartford, Connecticut.

He was a pastor, university professor, and lecturer. He attended Trinity College, graduating in 1855. He continued his studies, receiving his M.A. in 1859 and LL.D. in 1905 also from Trinity College. He obtained a degree of Doctor of Sacred Theology from Tufts College in 1880. He served as pastor of congregations in New England, New York, and Louisiana, leaving the South following the outbreak of the Civil War. In 1889, he began lecturing at the Tufts Divinity School. An entertaining lecturer, he presented a series of talks on London. He also lectured on microscopy at the Society for Natural History in Boston. He was made the first chaplain of the Tufts in 1905. He established a private collection of rare books, pamphlets, and maps, pertaining to the history of London. He amassed much of his collection while living in London during the 1870s. After his death, the collection was purchased by the trustees in 1921 for $1,400 and was given to the college's library as a memorial to the late professor.

In 1856, he married Mary D Waters (d. 1862). In 1863, he married Margaret A Barstow. He died on January 11, 1920, in Medford, Massachusetts.