Voluntown is a town in New London County, Connecticut, United States. The population was 2,603 at the 2010 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". Later land holders included Benedict Arnold, the Maj. General who later conspired unsuccessfully to turn over the plans of West Point, New York to the British and who betrayed his countrymen by leading British troops in battle against them.