Charlotte was born in Baltimore, Maryland. She was born the second daughter of nine children from her parents Charlotte and Thomas Stearns. Her father, Thomas, was a merchant who attempted living in different cities, before he settled down as a merchant partner in the trading firm of Stearns & Bailey in Boston, Massachusetts. Charlotte attended private school and graduated from the advance class of the State Normal School of Framingham, Massachusetts in 1862. She was employed as a teacher at a private school in West Chester, Pennsylvania. Her teaching career led her to Pennsylvania, Milwaukee at Antioch College and then back to Framingham and then to the St. Louis Normal School in St. Louis, Missouri.
Stearns married Henry Ware Eliot (1843 – 1919) on October 27, 1868, in Lexington, Massachusetts. They returned to Eliot's home city of Saint Louis, Missouri where they worked and reared their family. They had five daughters and two sons: Ada (Eliot) Sheffield, born in 1869; Margaret Dawes Eliot, born in 1871; Charlotte (Eliot) Smith, born in 1874; Marian Cushing Eliot, born in 1877; Henry Ware Eliot, Jr., born in 1879; Theodora Sterling Eliot, born in 1885 but died in infancy, and Thomas Stearns Eliot (T.S. Eliot), born in 1888. Charlotte's youngest child inherited his mother's literary skills and became the poet known as T. S. Eliot. In the 1870s when her husband hit bankruptcy, Charlotte taught school at the nearby Mary Institute
Thomas Stearns Eliot (T.S. Eliot) was born in St. Louis, Missouri in 1888. The Eliot family, including his mother Charlotte, his father Henry and T.S.'s six other siblings resided at 2635 Locust Street in St. Louis, Missouri. Eliot attended Smith Academy and then furthered his education at Harvard University in Cambridge, Massachusetts. When T.S. was at Harvard, Charlotte sent him the following letter:
"I hope in your literary work you will receive early the recognition I strove for and failed. I should so have loved a college course, but was obliged to teach before I was nineteen. I graduated with high rank, 'a young lady of unusual brilliancy as a scholar' my old yellow testimonial says, but when I was set to teaching young children, my Trigonometry and Astronomy counted for nought, and I made a dead failure."
Charlotte was a teacher for several years before she was a scholar and a writer of poems. Many of her poems appeared in religious periodicals. A collection of her poems, Easter Songs, was published in 1899. Her dramatic poem, Savonarola, was published in 1926 with the help of her son, T.S. Eliot. She was interested in the dramatization of events from medieval and Renaissance history that reflected the struggles of men who died for their faith. Charlotte's tone in her poetry was that of a dignified passion.
After her years as a teacher, she participated in social reforms including providing a house of detention for juveniles.
She also wrote a biography of her father-in-law, William Greenleaf Eliot, a Unitarian minister and leading citizen of St. Louis titled, William Greenleaf Eliot: Minister, Educator, Philanthropist (1904).
Charlotte left St. Louis and moved to Cambridge, Massachusetts after the death of her husband in 1919. Charlotte died in Cambridge in 1929 at eighty-six of a cerebral thrombosis. After her cremation, her ashes were buried next to her husband's plot in Bellefontaine Cemetery in St. Louis. After Charlotte's death in 1929, Henry Ware Eliot Jr. placed her poems and literary work in the Eliot collection at Harvard University.