- Admiral John Randolph Tucker Papers, 1865/18971
- Alexander Haight family collection, 1764/19762
- Alexander Haight family collection, 1764/19773
- Alexandria Gazette Ledgers (MS026), 1833/18661
- Alexandria History Collection (MS240), 1767/200815
- Alexandria Library Company Records (MS002), 1794/20074
- Allen Family Papers, 1766/19335
- Allen-Johnson Family Papers, 1838/19471
- Alumni Association Records, 1833/2014, bulk 1950/20052
- Ancella Bickley, Historian, Research Papers regarding African-Americans, 1775/2018, bulk 1970/20112
- Anna Maria Hickman Otis Mead Chalmers family papers, 1821/18974
- Appalachian Prints Collection, 1839/2010, bulk 1859/19092
- Armistead-Cocke Papers, 1680/19172
- Arthur I. Boreman Papers, 1830/19492
- Atkeson-Morgan Family Papers, 1833/1923, bulk 1850/19008