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Carroll was the only Roman Catholic to sign the Declaration of Independence. He added "of Carrollton" to his signature to separate himself from the other Charleses in his sprawling family – including his father, Charles Carroll of Annapolis. Charles was diminutive in stature, he was graceful in his movements and an accomplished horseman and he had fine, regular features. Charles was often described as the richest man in the country.

Educated in his early years by Jesuits, he spent many years in school in Europe and having studied law in Paris and London he was an unusually cultivated young man. After his marriage he lived the life of a landed gentlemen on Carrollton Manor, a ten thousand acre plantation in Frederick County, Maryland which he had received from his father. Not until he was thirty-six in 1773, did he become a public man. He was instrumental in asking Canada to help America in the Revolutionary War. He was elected to Maryland's first state senate in 1777. From 1776 to 1778 he was a member of the Continental Congress, where he signed the Declaration of Independence. He was a U.S. Senator from Maryland between 1789 and 1792. He retired from politics in 1800 but lived until 1832, being the last surviving Signer when he died at the age of ninety-four. Four years before his death, he officially opened the Baltimore and Ohio Railroad thus becoming the only Signer who ever saw a steam locomotive. Still regarded as the richest man in the country, he had long been a legendary figure.⁷