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Four of his uncles James, Edward, Robert and Francis Grimston all played first-class cricket, as did his cousin Walter Grimston.
Rev. Hon. Francis Sylvester Grimston (1822–1865), married Katherine Morier and had issue
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In 1802 Grimston was elected to the House of Commons for St Albans, a seat he held until 1808, when he succeeded his father as fourth Viscount Grimston and second Baron Verulam and entered the House of Lords.
He died in December 1773, aged 62, and was succeeded in his titles by his son James.
He died 1780, when the 3rd Viscount Grimston, his daughter's husband, succeeded him here.