Brooke was born at Colebrooke Estate, County Fermanagh, the son of Sir Arthur Brooke, 2nd Baronet, an Ulster aristocrat and his wife Julia Henrietta née Anson in the north of Ireland and succeeded to his title and the Colebrooke Estate in 1854.
William Flower was first introduced to him in India by Edward Blyth in 1870 and wrote on Brooke's contributions to natural history.
Brooke married Alice Sophia, daughter of Sir Alan Edward Bellingham, 3rd Baronet, who he met at a party, in 1864.
Another son served in India as a military secretary to The 4th Earl of Minto, Victor Reginald Brooke (1873-1914), and took a keen interest in hunting.
Brooke died of pneumonia in Pau in November 1891, aged 48, and was succeeded in the baronetcy by his eldest son, Arthur.