He was president of the Alabama Senate when Governor Gabriel Moore was elected to the United States Senate, and so became governor when Gabriel Moore resigned to take the seat.
He served as president of the Senate in 1831 when he succeeded Gabriel Moore.
Like his predecessor, Samuel Moore continued to survey the Coosa River through The Board of Internal Improvement, build infrastructure, and oppose nullification.
Moore strongly supported the Bank of the State of Alabama.
Moore died in 1846 at age 57 and is interred at the city cemetery in Carrollton in Pickens County.