Smith published the first of several school dictionaries in 1850, and in 1853 began the
Principia series, which marked an advance in the school teaching of Greek and Latin. Then came the ''Student's Manuals of History and Literature'', of which the English literature volume went into 13 editions. He himself wrote the Greek history volume. He was joined in the venture by the publisher
John Murray when the original publishing partner met difficulties. Murray was the publisher of the 1214-page
Latin–English Dictionary based upon the works of Forcellini and Freund that Smith completed in 1855. This was periodically reissued over the next 35 years. It goes beyond "classical" (100 BCE – 100 CE) Latin to include many entries not found in other dictionaries of the period, including
Lewis and Short. Perhaps the foremost books Smith edited covered ecclesiastical subjects: the
Dictionary of the Bible (1860–1865), the
Dictionary of Christian Antiquities (1875–1880), jointly with Archdeacon
Samuel Cheetham, and the
Dictionary of Christian Biography (1877–1887), jointly with
Henry Wace.
The Atlas, on which Sir
George Grove collaborated, appeared in 1875. From 1853 to 1869 Smith was classical examiner to the
University of London, and on retirement he became a member of the Senate. He sat on the Committee enquiring into questions of copyright and was for several years registrar of the
Royal Literary Fund. He edited
Gibbon, with
Guizot's and
Milman's notes, in 1854–1855. ==Honours and death==