After serving as governor and being succeeded by his handpicked man John Murphy, Pickens was appointed to the United States Senate to fill the vacancy left by the death of Henry H. Chambers, whom he beat twice for the governorship.

He only served from February 17 to November 27, 1826, when the elected successor, John McKinley, took office.

In addition to politics, Pickens participated in the American Colonization Society and was interested in scientific research.

He was originally buried in a family graveyard, but his remains were later moved to City Cemetery, Greensboro, Alabama.

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