The Cherohala Skyway— a National Scenic Byway completed in 1996— traverses the crest of the Unicoi Mountains connecting Tellico Plains, Tennessee with Robbinsville, North Carolina.

It refers to the low-lying clouds and fog that often drape the Southern Appalachian mountains in the early morning or on humid or moist days.

Another tributary of the Little Tennessee, Citico Creek, is formed by the convergence of two streams which rise in a densely forested area of the northwestern Unicois known as Jeffrey Hell.

The Unicoi Mountains consist chiefly of Precambrian metasedimentary rocks of a type known as the Ocoee Supergroup, formed over a billion years ago from ancient ocean deposits.

The Unicoi Mountains were formed roughly 250 million years ago during the Alleghenian orogeny, when a continental collision thrust the rocks upward.

[4] While the vast majority of trees in the Unicoi Mountains are second-growth, the range is home to one of the few remaining stands of old-growth forest in the eastern United States.

Grassy balds—a type of highland meadow consisting of fields of thick grass and sparse tree coverage—are not uncommon in the higher elevations.

Known as the Wachesa Trail (after a later Cherokee who lived at its eastern terminus), the path stretched from modern Cowee to a halfway point near Beaverdam Creek and descended through Unicoi Gap to Great Tellico.

In 1540, the Hernando de Soto expedition passed just west of the mountains en route from the Chiaha villages in East Tennessee to the Coosa chiefdom in northern Georgia.

Chicken, a South Carolina emissary travelling to the Overhill towns in hopes of obtaining their support in the colony's ongoing struggles with the Creek tribe, left Little Tellico in the Middle towns at 10am on July 24, 1725 and proceeded approximately 25 miles (40 km) across the southern Unicois to a campsite "about five Miles Short of a place called the Beaver Dam."

Chicken's party departed at 5am the following morning and arrived at the village of Great Tellico at 3pm, having travelled another 25 miles (40 km).

Cuming followed the same trail Chicken had taken five years earlier, departing from Tassetchee in the Middle towns and proceeding to a campsite "3 miles from Beaver Dam Creek."

The following day, Cuming's party passed over "Ooneekawy Mountain" and proceeded another 12 miles (19 km) to Great Tellico.

Stratton lived just west of the mountain's summit in a meadow now known as "Bob Bald" until 1864, when he was ambushed and killed by bushwhackers at the height of the U.S. Civil War.

[11] Sometime after the Civil War, the family of John and Albertine Denton moved to Little Santeetlah Creek, where they built a log cabin.

[12] Around 1911, George Gordon Moore— an official for the Whiting Manufacturing Company— attempted to establish a boar hunting reserve atop Hooper Bald in the southeastern Unicois.

[13] Moore attempted the same feat at his Rancho San Carlos in Carmel, California which had the same results of invasive wild boar escaping and devastating the local landscape.