Smith starred alongside such screen legends as leading ladies Greta Garbo, Elizabeth Taylor, and Vivien Leigh and the actors Clark Gable, Laurence Olivier, Ronald Colman, Maurice Chevalier, and Gary Cooper. His films include such classics as The Prisoner of Zenda (1937), The Four Feathers (1939), Hitchcock's Rebecca (1940), Dr. Jekyll and Mr. Hyde (1941), And Then There Were None (1945) in which he played General Mandrake, and the 1949 remake of Little Women starring Elizabeth Taylor and Janet Leigh, in which he portrayed the aged grandfather of Laurie Lawrence, (played by a young Peter Lawford), who generously gives a piano to the frail Beth March (played by Margaret O'Brien). He also appeared as the father of Maureen O'Sullivan in Tarzan the Ape Man, the first Tarzan film with Johnny Weissmüller. Smith also played a leading role as the Earl of Dorincourt in David O. Selznick's literature adaption Little Lord Fauntleroy (1936).