In 1839 he gained a diploma of the Royal Society of Antiquaries of Copenhagen for his work The Northmen in New England, or, America in the Tenth Century while his interest in geology and subsequent papers led to him being offered the position of President of the newly formed Geologists' Association, but other than delivering the inaugural speech, he did very little.
However, the main focus of his writings for many years was as a proponent of local self-government through traditional institutions, such as the parish, the vestry and the ward, a subject also taken up by his daughter Lucy Toulmin Smith.
After the cholera epidemic of 1847, Smith's knowledge of law combined with his involvement in his own Highgate neighbourhood led to his demanding better sanitation and reforms advocating devolution and local responsibility.
[3] This view was based in part on interpretation of medieval documents such as the Domesday Book (a survey of property in England compiled under the orders of William the Conqueror in 1086).
For example, Smith gave much space and enthusiasm to a project in 1861 to reproduce Domesday Book as individual counties using a new photographic process called photozincography under the supervision of Sir Henry James at the Ordnance Survey.