- Anna Jarvis (1864-1948) Papers, 1858/19581
- Anna Maria Hickman Otis Mead Chalmers family papers, 1821/189721
- Anne Atkinson Chamberlayne Collection., 1742/19632
- Anne McClung Collection, 1844/19661
- Annual and special reports of the Superintendent, 1840/19941
- Anson Du Puy Van Buren letters, 1863/19971
- Anthony Ware, Miscellaneous Papers, 1773/18861
- Antoine Gaujot and Julien E. Gaujot Papers, 1840/19992
- Appalachian Prints Collection, 1839/2010, bulk 1859/190910
- Appomattox Manor Music Collection, 1800/1940, bulk 1850/19101
- Arah J. Evans Autograph Album, 1849/19531
- Archer Lawrie Sheet Music Collection, 1879/19351
- Archer and Schuyler Bland Family Papers, 1870/18901
- Archibald W. Campbell (1839-1899), Newspaperman, Papers, 1855/1941, bulk 1855/18993
- Aretas Brooks Fleming (1839-1923) Papers, 1784/19241