In September 1853 Alford moved to Quebec Street Chapel, Marylebone, London, where he had a large congregation. In March 1857 Lord Palmerston advanced him to the deanery of Canterbury, where, till his death, he lived the same energetic and diverse lifestyle as ever. He had been the friend of most of his eminent contemporaries, and was much beloved for his amiable character. The inscription on his tomb, chosen by himself, is "Diversorium Viatoris Hierosolymam Proficiscentis" ("the lodging place of a traveler on his way to Jerusalem").