Greenville is a town in Orange County, New York, United States, located along the southern county and state line. The population was 4,689 at the 2020 census. Greenville has neither cities nor villages, and most of the communities are small clusters of houses. Greenville is near Exit 4 off Interstate 84, which features the town's firehouse and a few other bu…Greenville is a town in Orange County, New York, United States, located along the southern county and state line. The population was 4,689 at the 2020 census. Greenville has neither cities nor villages, and most of the communities are small clusters of houses. Greenville is near Exit 4 off Interstate 84, which features the town's firehouse and a few other businesses.