In 1802, Smith was elected to the United States Senate from Vermont, and served in the Senate from 1803 to 1807. In 1807 he successfully ran against one of his old political rivals, Isaac Tichenor, for governor. Tichenor had served as governor for a decade. Smith resigned from the Senate and served as Governor of Vermont from 1807 to 1808, when he was defeated for reelection by Tichenor. Smith served as Vermont's fourth Governor.
