According to James Mooney, his Cherokee name was "Ata'-gul-kalu", which could be translated "leaning wood", from "ata" meaning "wood", and "gulkalu", a verb that implies something long and unsupported, leaning against some other object. His name "Little Carpenter" came from a maternal ancestor, Thomas Pasmere Carpenter, and Englishman of Norman descent.
Family tradition maintains that he was born on Seivers Island (near Chota) around 1708 to Nancy Moytoy (eldest daughter of Moytoy I b. 1683) and her husband Moytoy IV. Moytoy IV was an Algonquin named White Owl Raven Carpenter (also called Raven of Chota) who had been adopted by Moytoy II (Trader Tom Carpenter). He married Nionne Ollie, who was the daughter of his cousin Oconostota (the marriage was permissible because they were of different clans; he was Wolf Clan and she was Paint Clan). Among their children were Dragging Canoe and Dutsi, through whom Major Ridge and David Watie were grandchildren of Attacullaculla.
He was a member of the Cherokee delegation that traveled to England in 1730. In 1736, he rejected the advances of the French, who sent emissaries to the Overhill Cherokees. Three or four years later, he was captured by the Ottawa, allies of the French, who held him captive in Canada until 1748. Upon his return, he became one of the Cherokees' leading diplomats and an adviser to the Beloved Man of Chota.
In May 1759, following a series of attacks by settlers and Cherokees against each other, Attacullaculla joined a delegation that went to Charleston to try to negotiate with South Carolina authorities. Governor William Henry Lyttleton seized the delegates as hostages until the Cherokees responsible for killing white settlers were surrendered. Having raised an expeditionary force, Lyttleton set out for Fort Prince George with the hostages in tow and arrived with 1700 men on December 9, 1759. Though freed soon after, Attacullaculla returned to Fort Prince George to negotiate for peace, but his efforts were thwarted by the more hawkish Oconostota. The Cherokees gave up two individuals and negotiated the release of a few hostages including Oconostota, who soon after lured Lt. Richard Coytmore out of the fort, waving a bridle over his head, and incited Cherokee warriors hiding in the woods to fire upon and kill Coytmore; white soldiers inside the fort then proceeded to murder all the Cherokees inside, and hostilities continued between the Cherokees and Anglo-Americans.
His death is believed to have occurred either in 1775 or 1777, after which he was succeeded by his cousin, Oconostota (who was also his father-in-law). Attacullaculla did not use the European title "Emperor of the Cherokees" that his uncles had.