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He was governor and heir-apparent to the proprietorship of the colony; married the widow of his close friend Henry Sewall, who immigrated with him in 1661 when both established a residence at Mattapany. Governor of Maryland, 1661-1675; Secretary, 1665-1666, 1667-1669, 1673-1673/74; Collector of Patuxent, 1673-1675/76; proprietor of Maryland, 1675-1714/15 (without governing rights, 1689-1714/15).

He expressed frequent discontent in the 1660s and the 1670s with the caliber and social standing of the Council and was often at odds with his uncle Philip Calvert (1626-1682) and the latter's protegee, Henry Coursey (ca. 1629-1695). He continued his father's policy of religious toleration, and in particular reached accommodation in the 1680s with the Quakers; fashioned a close circle of political leaders, almost exclusively Catholics, who were usually bound to him by blood kinship or marriage, especially in the case of his Sewall stepchildren; his struggles with William Penn over the northern boundary of Maryland and attacks against the colony's charter finally necessitated his return to England in 1684; his deputies lacked Calvert's ability to defuse attacks and govern smoothly; Calvert lost his colony in the royal settlement following the Glorious Revolution, during which he was charged with outlawry and treason, charges that were later dropped. He made many unsuccessful efforts to regain the colony over the subsequent twenty-five years and he broke off relations with his son Benedict Leonard Calvert, 4th Lord Baltimore (1679-1715) upon the latter's conversion to Protestantism.

When he was about fourteen years old he graduated from Oxford University, and after spending a few years in travel he was made Clerk of the Privy Council and later secretary of state. While holding the latter office he won the favour of James I., by whom he was made a knight in 1617, and in 1625 created Baron Baltimore of Baltimore, Ireland. It was also from the hands of this monarch that he received his grant of the province of Avalon in southern Newfoundland, where he founded a colony, which he visited, but did not remain on account of the extreme cold. After visiting the southern part of the American coast, he urged Charles I. to grant him another patent, consisting of the tract of land now covered by Maryland and Delaware. Lord Baltimore intended to found a state which should be governed by an assembly, and should have an hereditary landed aristocracy.