After education at Enfield he entered St. Bartholomew's Hospital in 1832, being apprenticed to Frederic Carpenter Skey, with whom he lived, and whose house surgeon he afterwards became.
On his return to England he was appointed surgeon to the Royal General Dispensary in Aldersgate Street, and he also lectured on surgery at Samuel Lane's school of medicine in Grosvenor Place.
Caring little for private practice, Smith gave both time and thought to the welfare of the newly founded St. Mary's Hospital and its medical school.
His library, rich in medical works of the sixteenth and seventeenth centuries as well as in editions of Thomas a Kempis and of Izaak Walton's The Compleat Angler, was sold by Messrs. Sotheby, Wilkinson, and Hodge on 14, 15, and 16 Nov. 1878, and on 17 and 18 June 1897.
Smith translated from the German, for the Sydenham Society, Dr. Theodor Schwann's 'Microscopical Researches into the Accordance in the Structure and Growth of Animals and Plants' (1847) and Dr. M. J. Schleiden's 'Contributions to Phytogenesis' (in the same volume).