Styled Marquess of Tullibardine from birth, he was born at Blair Castle, Perthshire, the second but eldest surviving son of John Stewart-Murray, 7th Duke of Atholl, by Louisa, daughter of Sir Thomas Moncreiffe of that Ilk, 7th Baronet. and was educated at Eton College. He learned to speak Gaelic before English. In "Working Partnership" his wife, The Duchess of Atholl, says that Tullibardine and all his siblings were brought up to speak Gaelic and were "extremely proficient" in it. He was President of An Comunn Gàidhealach, the national Gaelic Society, from 1898 until 1904.
He was commissioned into the Royal Horse Guards with the rank of second lieutenant on 28 December 1892, and was promoted to lieutenant on 30 December 1893. He served in Kitchener's expedition to the Sudan, fighting at the Battle of Khartoum and the Battle of Atbara. He was awarded the Distinguished Service Order on 15 November 1898, and rose to the rank of captain a year later, on 20 November 1899.
In 1900 he served as an aide-de-camp to Brigadier-General J. F. Burn-Murdoch, in command of a brigade of the Cavalry division stationed in Natal. In November 1900 he was given the rank of brevetmajor in the Royal Horse Guards, and asked by Lord Kitchener, whom he had served under on the Omdurman Campaign, to raise a regiment of Scotsmen in South Africa, called The Scottish Horse. The regiment was raised quickly and soon saw active service in the Western Transvaal. A second regiment of Scottish Horse was raised from troops recruited by The 7th Duke of Atholl and a permanent headquarters was set up to supply both of these regiments, with Atholl in command but with subordinate commanding officers in the field in charge of each of the Regiments. This success continued until the Scottish Horse was a whole brigade by the end of the Second Boer War. In August 1901 Lord Tullibardine received the local rank of lieutenant colonel in South Africa while commanding the Scottish Horse. He was mentioned in despatches by Lord Kitchener dated 23 June 1902. Following the end of the war in June 1902, Lord Tullibardine and most of the men of the Scottish Horse left Cape Town on the SS Goth in early August, and arrived at Southampton later the same month. After his return to the United Kingdom, he was on 28 September 1902 received at Balmoral Castle by King Edward VII, who presented him with the Insignia of a Member of the Royal Victorian Order for his services in South Africa. The following year he was promoted to the substantive rank of lieutenant colonel in the Army.
During the Second World War, despite being seventy years old, Atholl joined the Home Guard and reportedly took turns as sentry officer on duty in Whitehall. He remained closely involved with the Scottish Horse, remaining in the post of Colonel Commandant until 1919 and Honorary Colonel from 1920 until his death in 1942. He was key in establishing a Scottish National War Memorial in Edinburgh Castle after the First World War and his papers relating to this are retained by the National Library of Scotland.
In 1932 Atholl came to national attention when he launched a lottery in an attempt to stop money going overseas to the Irish Free State Hospitals Sweepstakes. The money this scheme raised was given to British charities, mainly hospitals, but in 1933 he was prosecuted by the Director of Public Prosecutions, Sir Edward Hale Tindal Atkinson, for promoting an unlawful lottery. Despite this, Atholl's lottery activities were admired and seen by many British people as being patriotic.
Family life
While still Marquess of Tullibardine, Atholl married Katharine Ramsay, daughter of Sir James Ramsay, 10th Baronet, at St Margaret's Church, Westminster, on 20 July 1899. His wife went on to have a long political career in her own right in local government, in the House of Commons, and as a government minister. They had no children. Atholl died on 16 March 1942, aged 70, and was succeeded by his youngest brother, James Stewart-Murray. His widow, Katharine, Duchess of Atholl, died in October 1960, aged 85.