The park consists of 70 acres (28.3 ha) situated along the Sycamore Shoals of the Watauga River, a National Historic Landmark where a series of events critical to the establishment of the states of Tennessee and Kentucky, and the settlement of the Trans-Appalachian frontier in general, took place.

Richard Henderson and Daniel Boone negotiated the Treaty of Sycamore Shoals in 1775, which saw the sale of millions of acres of Cherokee lands in Kentucky and Tennessee and led to the building of the Wilderness Road.

During the American Revolution, Sycamore Shoals was both the site of Fort Watauga, where part of a Cherokee invasion was thwarted in 1776, and the mustering ground for the Overmountain Men in 1780.

Adjacent to the fort is a 450-seat amphitheater, which is the site of the Official Outdoor Drama of the State of Tennessee, Liberty: The Saga of Sycamore Shoals (formerly billed as The Wataugans).

Listed on the National Register of Historic Places and built between 1775 and 1780, the Carter Mansion may be the only surviving material link to the Watauga Association and is the oldest frame house standing in Tennessee.

[3] In 1770, James Robertson (a later founder of Nashville) made an excursion into the Watauga Valley, possibly to locate settlement sites for families fleeing the turmoil of the Regulator Movement in his native North Carolina.

[9] In March 1775, the Treaty of Sycamore Shoals, sometimes called the Transylvania Purchase, was signed by Richard Henderson and Cherokee leaders Attakullakulla and Oconastota.

[4] In the weeks following the Treaty of Sycamore Shoals, a faction of Cherokee opposed to the sale, led by Dragging Canoe, aligned themselves with the British with plans to drive the settlers back across the Appalachian Mountains.

Overmountain Men had previously fought at the Siege of Charleston (these included what one historian dubbed the first "Tennessee volunteers")[11] and the Battle of Musgrove Mill, both in 1780, and participated in two campaigns against the Cherokee, in 1776 and 1780.