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". 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.
According to the United States Census Bureau, the town has a total area of 39.8 square miles (103 km2). 38.9 square miles (101 km2) of it is land and 0.9 square miles (2.3 km2) of it (2.14%) is covered by surface water.
At the 2000 census there were 2,528 people, 952 households, and 702 families living in the town. The population density was 65.0 people per square mile (25.1/km2).