- Angela Boserman, Collector, Letter and Tuition Account from Randolph County, 1855/18611
- Anita Cutright Burnett, Collector, Papers, 1790/19351
- Ann Lettice Murdoch diary, 1841/18641
- Ann Smith Academy Papers, 1807/19101
- Anna Burton Ellett Collection, 1751/19321
- Anna Maria Hickman Otis Mead Chalmers family papers, 1821/189726
- Anne Atkinson Chamberlayne Collection., 1742/19631
- Anne McClung Collection, 1844/19662
- Annie Haseltine Judson Chiles Autograph Album, 1850/18541
- Annual and special reports of the Superintendent, 1840/19941
- Anthony Ware, Miscellaneous Papers, 1773/18861
- Antoine Gaujot and Julien E. Gaujot Papers, 1840/19992
- Antonia Ford letters, 1855/18592
- Appalachian Prints Collection, 1839/2010, bulk 1859/19096
- Appomattox Manor Music Collection, 1800/1940, bulk 1850/19101