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Founder member of the Royal Society, one of the earliest Freemasons, he was devoted to the causes of the welfare of Scotland, loyalty to his monarch, and in promoting the new experimental philosophy. He was experienced in negotiating affairs of state, and an intimate friend of King Charles II. The son of Sir Mungo Moray of Craigie in Perthshire, he was educated in Scotland and in France, probably a member of the Scottish regiment which joined the French army in 1633. He made a considerable reputation for himself and was favoured by Cardinal Richelieu. In 1641 he was recruiting Scots soldiers for the French, later becoming Colonel of the Scots Guards at the French court. He was knighted in 1643 by Charles I. He was captured by the Duke of Bavaria in November 1643 whilst leading his regiment into battle for the French, and whilst in prison until 1645 was lent a book on magnetism by Kircherus, with whom he entered into correspondence. He tried unsuccessfully to arrange the escape of Charles I in 1646, and in 1651 was engaged in negotiations with the Prince of Wales to persuade him to come to Scotland, thus beginning his long friendship with the future Charles II.
After a failed Scottish rising in the Highland in 1653, his military career was over and he went into exile, in Bruges in 1656, then Maastricht until 1659, where he led the life of a recluse but spent his time in scientific pursuits. It was at this time that many of his letters to Alexander Bruce were written. Late in 1659 he went to Paris and did much, by correspondence, to help prepare for the return of the King to England, especially in relation to religious matters. After the return he was active in promoting the best interests of Scotland and was given high office. He was also provided with rooms at Whitehall Palace, the King's London residence, which included a laboratory, as the King shared his scientific interests. It was Moray who was the chief intermediary between the Royal Society and the King, and other highly placed persons at the Court such as Prince Rupert and the Duke of York. More important than his scientific work for the Society were his powers of organisation and firmness of purpose in establishing it on a sound and lasting basis, including his efforts in obtaining the three founding Royal Charters and his attempts to put the Society on a sound financial footing. In 1670 he and Lauderdale quarrelled, leading to Moray withdrawing from politics. On his death in 1673 he was buried in Westminster Abbey by personal order and expense of the king.