Married (1752) to Frances Mary Buckworth (d. 1759). Married (1759) to Elizabeth Cochrane, Boswell's mother's cousin. He had two children from his first marriage, Fanny (b. ca. 1755, d. 1832) and Buckley (possibly b. 1752 in Weston, Somerset, d. 1827).1
He entered the 3rd Regiment of the Guards in 1749 and remained in that regiment until 1766 when he retired with the rank of Lt-Colonel.
According to Boswell, Lt-Col Gould participated in the Affair of St. Cast.2
Boswell first met Nathaniel Gould on December 03, 1762. During the following months he often dined with the Goulds, and enjoyed their company. Boswell especially seems to have taken a liking to the Colonel, and on January 8, 1763 mentioned the Colonel's charming indolence in his journal.