Not fitting in at his college in terms of social activity, he devoted himself mainly to antiquarian research and drawing.

[5] Whilst being a welcome guest in society, he was in fact a literary recluse, who made no effort to keep up with fashion in his dress.

[2] His artefact collection included the coat-of-arms from Cardinal Beaton's (Bethune's) house on the Cowgate in Edinburgh.

In 1823 he published his Ballad Book, which in 1880 was re-edited by David Laing, with additions from Sharpe's manuscripts.

To Laing's edition of William Stenhouse's notes to James Johnson's Scots Musical Museum (1853), he made some contributions.

It was followed in 1820 by an edition of Robert Law's Memorialls; or the considerable Things that fell out within the Island of Great Britain from 1638 to 1684, containing information on witchcraft and related topics.