Voluntown is a town in New London County, Connecticut, United States. The population was 2,570 at the 2020 census. Voluntown was part of Windham County from 1726 to 1881. The town was named for the English volunteers in the 1675 Indian wars (King Philip's War) who stayed to fight "and went not away". One of the original founders of Voluntown was Lieutenant Thomas Leffingwell, who secured the town's approval in the colonial legislature and surveyed its original layout. Maj. General Benedict Arnold, the infamous Revolutionary War turncoat was a landholder.