Montour Falls is a village located in Schuyler County, New York, United States. The population was 2,714 at the time of the 2020 census. A waterfall at the end of West Main Street gives the village its name. The name "Montour" is derived from Queen Catharine Montour, a prominent Native American woman of Seneca Indian heritage who lived at the v…Montour Falls is a village located in Schuyler County, New York, United States. The population was 2,714 at the time of the 2020 census. A waterfall at the end of West Main Street gives the village its name. The name "Montour" is derived from Queen Catharine Montour, a prominent Native American woman of Seneca Indian heritage who lived at the village site in the 18th century.