He served one term as representative of the at-large district of Alabama (1821–1823). Moore was one of four candidates in the running. Moore won with 67.57% of the vote. He served as Alabama's 1st district representative (1823–1829). In the 1823 election, he was the only candidate and won all 3,304 votes. In the 1825 election, he was one of two candidates, the other being Clement Comer Clay. Moore won with 71.12% of the vote.
He was elected Governor of Alabama unopposed in 1829, standing as a Jacksonian.[4] In 1831, two years into his four-year governorship, Moore resigned to seek a Class 3 spot in the Senate. In response to his resignation, Moore was replaced as Governor by Alabama Senate President Samuel B. Moore (no relation).
Following his loss to McKinley, Moore moved near Caddo Lake, Texas, in 1843. He died there on August 6, 1844, and was buried on the plantation of Peter Swanson.