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Molyneux's brother, Sir Vivian Molyneux, was a scholar, traveller and Royalist agent in the 1640s, and an uncle of Robert Earl of Caernarvon, Lord Lieutenant of Buckinghamshire.
He was present at the siege of Manchester in September 1642, and on 20 April 1643 was defeated by Captain Ashton at Whalley.
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He married the Lady Frances, eldest daughter of William, Marquis of Hertford, but had no children.