Searle was educated at Christ's Hospital, supported by a governor of the hospital, Samuel Hoare. He was elected to a scholarship at Pembroke College in 1848, graduating B.A. (10th wrangler) in 1851. He was then elected to a Fellowship. He was ordained deacon in 1854, and priest in 1855. He went on to be curate in Broughton, Hampshire in 1855, of Odell, Bedfordshire, 1856-1864, and of Earl Stonham, Suffolk 1864-1870. In 1870 he returned to Pembroke as a tutor, and also served as lecturer and Dean. In 1880 he was elected Master of Pembroke, a position he held until his death in 1902. Subsequently, many members of the Searle family attended Pembroke College including Charles Frederick Searle, William Cavendish Searle, Edward Alborn Searle, John Alborn Searle, Jonathan Charles Searle, Frederick Charles Searle, Frederick St. Leger Searle, Robert St. Leger Searle, Charles Stratford St. Leger Searle, P. Warham St. Leger Searle, Peter Malcolm Searle, Jeremy Lawrence and Geoffrey Francis William Searle.