Augustus Smith's papers contain correspondence, autograph manuscripts written by Smith while at Hamilton College and Wesleyan, a notebook (part of which records Smith's journey to Labrador in 1860) diplomas, civilian commissions, deeds, and photographs. The bulk of the material dates from the mid-1820's to 1860. It consists of personal correspondence between Smith and members of his family, former classmates and pupils. There is scientific correspondence between Smith and contemporary astronomers, mathematicians and meteorologists. Finally, there are many letters between Smith and various members of the Methodist-Episcopal Church.