Carroll was a voice for independence in Maryland. In 1772 he engaged in a debate conducted through anonymous newspaper letters and maintained the right of the colonies to control their own taxation. He was a member of Annapolis' first Committee of Safety in 1775. In early 1776, while not yet a member, the Congress sent him on a mission to Canada. When Maryland decided to support the open revolution, he was elected to the Continental Congress on July 4, 1776, and remained a delegate until 1778. He arrived too late to vote in favor of it, but was able to sign the Declaration of Independence. Throughout his term in Congress he served on the board of war.
He returned to Maryland in 1778 to help in writing a constitution and forming a state government. Carroll was re-elected to the Continental Congress in 1780, but he declined. He was elected to the state senate in 1781 and served there continuously until 1800.
When the United States government was created, the Maryland legislature elected him the first United States Senate. In 1792 Maryland passed a law the prohibited any man from serving in the State and national congresses at the same time. Since he preferred to be in the Maryland Senate, he resigned from the U. S. Senate on November 30, 1792.
Charles retired from public life in 1801, although he did help to create the Baltimore and Ohio Railroad in 1827. After Jefferson and Adams died, on July 4, 1826 he became the only surviving signer of the Declaration of Independence. He died in November 14, 1832 at Baltimore, Maryland.
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