In 1882, the community—originally "Walker's Mill"—was named for Schuyler George Walker, local mill operator, and the area's first postmaster.
In the late 19th and early 20th centuries, the town became a small industrial center with the establishment of a stone cutting plant for the area quarries of the Alberene Stone Company, which took the native and acid-resistant soap stone and milled the rock into flat table tops for labs and hospitals. The Great Depression essentially destroyed this industry and the area never fully recovered.
Schuyler was the birthplace and home of writer Earl Hamner, Jr. He is best known for the CBS television series The Waltons, which was based on his experiences of growing up the eldest child of a large rural family in depression era America. Earl and his mother and siblings attended Schuyler Baptist Church near their home-place. There are still a few of the members that knew them. The church still has services every Sunday and has made upgrades in its technology.
The region suffered greatly from the remnants of Hurricane Camille, which dumped two and three feet of rain in the area in August 1969. The flooding and landslides are a major weather event of the late 20th Century.