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The second son of James Blount, 6th Baron Mountjoy, Charles became the most notable of the later holders of the barony, inheriting the title in 1594 on the death of his unmarried elder brother William.
After the creation of the Southwest Territory in 1790, the territory's governor, William Blount, selected White's Fort as the territory's capital.
He was one of the managers appointed by the House of Representatives in 1798 to conduct the impeachment proceedings against Tennessee U.S. Senator William Blount.
He was appointed that year by territorial Governor William Blount to survey the boundary with the Cherokee nation established by the 1791 Treaty of Holston.
He embarked in the William Blount conspiracy in instigating the Cherokee and Creek Indians to aid the British in their attempt to conquer the Spanish territory in Louisiana in 1797.
Mountjoy married firstly, about Easter 1497, Elizabeth Say, the daughter and coheir of Sir William Say of Essenden, Hertfordshire, by whom he had a daughter, Gertrude Blount, who married, on 25 October 1519, Henry Courtenay, Marquess of Exeter, and was a lady in waiting to Queen Mary.