Charles's mother, Mary Lyman Eliot, was a descendant of Pilgrims who landed in Plymouth in 1631. His father was a treasurer of Harvard College, who served as mayor of Boston. His wife inherited a small fortune, but in the panic of 1857, the family became impoverished.

When Charles was teaching mathematics and chemistry at Harvard College, his five year appointment ended without reappointment. He married Ellen Peabody, and they stretched their savings to travel to Europe where he visited leading universities. After he declined a highly remunerative offer as an industrial executive because he wanted to concentrate in the field of education, he accepted appointment as professor of chemistry, becoming part of the newly forming faculty of the Massachusetts Institute of Technology. Professor Eliot wrote two notable articles published in 1869 in the Atlantic Monthly calling for the reform of American universities.

In the same year, Eliot was astounded to be elected president of Harvard University by a close but nevertheless decisive vote. Four days later his wife died, leaving two motherless boys. He was inaugurated as Harvard's president in the meeting house of the First Church (Unitarian) in Cambridge, where he remained a member for life. Eliot worked closely with the presidents of Cornell and Johns Hopkins—Andrew White and Daniel Colt Gilman—jointly to create a viable structure of higher education in America.

President Eliot was patient as well as persistent in the face of opposition as he boldly labored to unify the education system. He also gained world renown for his service as a citizen. Best remembered, other than for his presidency, are the five-foot series of 50 volumes in our libraries, The Harvard Classics, which he edited in retirement to advance education for people with a passion to learn.