William Cayley was born on 14 December 1836 in Stamford, Lincolnshire, England. He was educated at Shewsbury School, Queen's College, Cambridge and King's College, London (where he studied medicine). He had a distinguished career as a doctor and teacher of medical students at Middlesex Hospital and King's College Hospital. While his considerable medical skills were recognised, his obituary in The Lancet described him as "reticent to a fault and lacking in the bedside manner and the capacity for small talk that often contribute to popular success. A lover of flowers and the classics, he was an expert mountaineer, spending his annual holidays in Switzerland and the Tyrol. A bachelor, non-smoker and teetotaller, he died in retirement in Richmond." He died on 17 December 1916.
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