Brooke's accomplished poetry gained many enthusiasts and followers including Edward Marsh, who brought him to the attention of Winston Churchill, then First Lord of the Admiralty. Brooke was commissioned into the Royal Naval Volunteer Reserve as a temporary Sub-Lieutenant shortly after his 27th birthday and took part in the Royal Naval Division's Antwerp expedition in October 1914.

He sailed with the British Mediterranean Expeditionary Force on 28 February 1915 but developed sepsis from an infected mosquito bite. He died at 4:46 pm on 23 April 1915, on the French hospital ship, the Duguay-Trouin (named after the famous 17th century privateer, René Duguay-Trouin), moored in a bay off the Greek island of Skyros in the Aegean Sea, while on his way to the landing at Gallipoli. As the expeditionary force had orders to depart immediately, Brooke was buried at 11 pm in an olive grove on Skyros. The site was chosen by his close friend, William Denis Browne.

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