Smethport is located on a floodplain adjacent to Potato Creek, which empties into the Allegheny River. The John Keating Land Company, whose agent surveyed the site in 1807, donated land for the settlement. Keating chose to name it after his two Amsterdam bankers, Raymond and Theodore de Smeth. The village's development was delayed by its distance from the Allegheny River.
Solomon Sartwell, a New Hampshire builder, settled in Smethport in 1816. Protestant families from Connecticut moved here in the 1830s and 1840s. By 1853, the village was incorporated as a borough and a trading center for lumbermen, as well as being the county seat. The arrival of the railroad and the discovery of oil created a demand for housing. With little pressure for later development, the best of these houses remain intact. One of the reasons U.S. 6, also known as the Grand Army of the Republic Highway, is considered scenic is that it passes through this charming town. Additionally, the handsome courthouse ( MK1) and several substantial, high-style, late-nineteenth- and early-twentieth-century houses line Main Street, notably the former Charles McKean House (1904; W. Main and Mechanic streets) and the former Orlo Hamlin house (1900–1901; 911 W. Main Street), now adapted for apartments. Stylistically, the houses range from Queen Anne to Italianate, some have classical detailing, and several have cupolas. As would be expected in a timber area, more houses are of wood than of brick.
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