During the estate’s heyday, the Coach Barn stabled riding and carriage horses for the Webb family, stored their extensive collection of carriages, sleighs, harnesses, and saddlery, and housed groomsmen. Completed in 1902, it was the last major Shelburne Farms building designed by Robert H. Robertson, and the last major building constructed on the property. Robertson considered the Coach Barn—with its eyebrow windows, arched entrance and courtyard— his architectural gem A central, brick-floored washroom was flanked by storage rooms for carriages and tack, with additional storage rooms upstairs. Box stalls and hay lofts were located in the wings. When a call came down from the "Big House" for a carriage or saddle ride, grooms harnessed the horses then headed up the hill. By the 1910s, the Coach Barn also housed the Webbs’ growing fleet of automobiles.

In 1947, the Webb’s carriage collection and equipment were donated to the newly-formed Shelburne Museum. Today, many of them are on display in the Museum’s Horseshoe Barn. For the next 25 years, the barn continued to be used for agricultural purposes: housing sheep, wintering heifers and hosting cattle auctions. After descendents formed the nonprofit environmental education organization in 1972, the Coach Barn served as an education center, the site for school trips, summer camps and educator workshops.