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Lord George was the son of John Murray, 1st Earl of Atholl. Along with two of his brothers, Murray joined the Jacobite uprising in 1715. Following its defeat in 1716, Murray fled to the Continent. He also took part in the invasion of Scotland in 1719.
He was pardoned in 1725 and raised a family on a country estate in Scotland, outwardly appearing to be a government supporter. However, when Charles Edward Stuart landed in Scotland in 1745, Murray went over to the Jacobite side and was appointed lieutenant-general in Charles's army. He played a large part in the defeat of General Cope's army at Prestonpans in September 1745.
Murray led the Jacobite army south through England to Derby, but was pessimistic about the chances of further success. He persuaded Charles to retreat on 6 December 1745. Murray led the right wing at the Battle of Falkirk in January and defeated Hawley's forces. He strongly advised against joining battle at Culloden in April 1745, but fought on the right wing. The day after the defeat, Murray resigned his command and wrote a reproachful letter to Charles.
After a period in hiding, he escaped to the Continent, where he remained in exile for the rest of his life.