In 1806, he became a candidate for the office of Secretary to the Society of Antiquaries, which he obtained the following year.
In 1812, he became an Assistant Librarian of the Royal Library; he went on to accompany that collection to the British Museum, which he attended two days each week.
He also wrote an historical account of Charitable Commissioners, and of Foreign Orders of Knighthood.
His father married, first, Elizabeth Hutchinson; they had at least one child, a son, the surgeon, Anthony Carlisle.
Carlisle entered the naval service of the East India Company, attaining the post of purser.