In 1832, Moore's daughter, Elizabeth, married Clement Finley, who later became the tenth Surgeon General of the United States Army.

Moore was elected as a Republican to the Fifteenth Congress to fill the vacancy caused by the resignation of Samuel D. Ingham.

He then served as chairman of the United States House Committee on Indian Affairs during the Seventeenth Congress.

He was appointed by President James Monroe as director of the United States Mint on July 15, 1824, holding this office until 1835.

Moore moved to Philadelphia, Pennsylvania, where he became interested in the mining and marketing of coal, serving as president of the Hazleton Coal Company until his death in Philadelphia in 1861.