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In 1848, Cohoes was incorporated as a village within the town of Watervliet. In 1869 it was chartered as a city.

Harmony Mill No. 3, in 1969

Map of the village of Cohoes in 1866. North is to the right.

Map of Cohoes in 1891

In 1866, during excavation work for construction of Mill #3 of the Harmony Mills, the bones of a mastodon were unearthed over a period of several weeks. This mammal ranged in this territory when humans were first settling here. The Cohoes Mastodon skeleton was long on display in the lobby of the New York State Museum in Albany, New York. Since the early 21st century, the skeleton has been moved to a new location away from the windows, where temperature and humidity fluctuations risked damaging the skeleton. A replica complete with fur is on display at the Cohoes Public Library.
Upon their completion, in 1872, the Harmony Mills were the largest cotton mill complex in the world. The Harmony Mills are an excellent example of 19th-century mill architecture. During the 19th century, numerous immigrants came to Cohoes to work in the mills, particularly French Canadians from Quebec and Irish, who first arrived as refugees in the 1840s from the Great Famine.The Harmony Mills Historic District was listed on the National Register of Historic Places in the late 20th century.
Around the start of the 20th century, daredevil Bobby Leach practiced going over the Cohoes Falls in a barrel before he performed the same stunt at Niagara. Cohoes residents watched this feat from the lawn or the porch of The Cataract House, the Victorian hotel at the corner of North Mohawk and School streets. This site was later developed as the present School Street Power Station.
In 2005-2013, the Harmony Mills were redeveloped and restored by real estate developer Uri Kaufman. Kaufman converted the Mills to luxury loft apartments, sparking a revival in the heart of the City.