 He completed his medical training at Guy's Hospital in London.In 1900, as part of the British efforts during the Boer War, he travelled to South Africa and worked as a dresser in the Imperial Yeomanry Hospital under Dr Alfred Fripp.Ayre-Smith played club rugby for Guy's Hospital, and in 1899 he was selected to join Matthew Mullineux's British Isles team on the first official tour of Australia.