A rural community in Windham County, Pomfret was purchased from the Indians in 1686. Major Fitch, acting as agent for Owaneco, and the purchasers arranged for the conveyance. The price was 30 pounds and was known at that time as "The Mashmuket Purchase". Mashamoquet, the name first applied to the largest stream which runs through Pomfret, was signified by the Indians as a great fishing place. The area at that time was about 18,270 acres.

    The first settler was probably Captain John Sabin who built a house in 1696. His home also served as an outpost against the Indians. The Mashamoquet Brook was a source of power for small mills which developed along it and its tributaries. The ruins of these mills and their dam foundations still exist along the brook. The written evidence of these mills is found in Pomfret's land records. An example of one of these mills, the Brayton Grist Mill, stands at the entrance of Mashamoquet State Park on Route 44 and is open to visitors.

    Pomfret is probably best known for the wolf's den where General Israel Putnam killed the last wolf in Connecticut. Wolf Den is now maintained as a state park and has been placed on the National Register of Historic Places by the National Park Service.

    The Mashmuket Purchase was incorporated by legislature and called Pomfret in 1713. The name of the town was derived from the town of Yorkshire (Pontefrat, pronounced 'Pomfret') which was the English home of the family of Governor Saltonstall. In the ensuing years Brooklyn became a town, Hampton became a town and in 1855 Putnam became a town. All of these new towns took land from Pomfret. That portion lost to Putnam was by far the most damaging economically as it included a section known as Pomfretville or what today is known as the Cargill Falls. Pomfretville or Pomfret Factory was the industrial center of Northeastern Connecticut at that time.

    Today Pomfret has much open land as result of Mashamoquet Brook State Park, and the efforts of the Connecticut Audubon Society, the Wyndham Land Trust as well as the Department of Environmental Protection. Pomfret buildings and sites on the National Register of Historic Places include the Brayton Grist Mill, the Abington Congregational Church, Wolf Den, the Old Town House and most recently Pomfret Street Historic District. On the State Register of Historic Places is the Averill-Hotchkins house.

    Pomfret has experienced a change from being strictly rural agricultural to being rural residential with approximately 14 farms left of which 5 are dairy farms. The others range from apple and grape orchards to pumpkins. Pomfret also supports several thriving worldwide industrial complexes ranging from fiber optics to forest products.