He was born at Kingston Hall, in Somerset County, Maryland on April 29, 1793, the son of Col. Henry James Carroll and Elizabeth (Barnes) King.

Carroll studied law, first in the office of Ephraim King Wilson in Snow Hill, then under Robert Goodloe Harper in Baltimore.

While governor, he joined in the movement to improve the collegiate department of the University of Maryland, as well as that of advocating a statewide public school system.

Carroll retired to Kingston Hall at the close of his administration and lived there until 1840, when he moved to Dorchester County, Maryland, residing on a large estate near Church Creek.

He died at his home Walnut Landing, in Dorchester County on October 3, 1873, and was buried in Old Trinity Church Cemetery following Masonic burial services.