Smith is considered to be the first Englishman to be a serious antiquarian and musicologist. He began by publishing "A Collection of English Song" in 1779, which musicologist Nicholas Temperley called "perhaps the first scholarly edition printed in England." Smith's library included the "Old Hall Manuscript", Drexel 4175, as well as a copy of "Ulm Gesangbuch" from 1538 that had belonged to Johann Sebastian Bach. He also collected works that dated back to the 12th century including some Gregorian chants. His publication "Musica Antiqua" (1812) included musical scores of works by Jacob Obrecht, Adrian Willaert, Jacob Clemens and Cristóbal de Morales with historical notes on each piece. According to Vincent Duckles, Smith's major contribution was "to direct the attention of his readers to the importance of source studies."