- Alexander, Fultz, and Willson Families Collection, 1770/19701
- Alexandria Gazette Ledgers (MS026), 1833/18661
- Alexandria History Collection (MS240), 1767/20081
- Alexandria Library Company Records (MS002), 1794/20071
- Alexandria Scrapbook Collection (MS003), 1830/18931
- Alexandria, Virginia City Records (MS019), 1750/1983, bulk 1825/18751
- Alfred Beckley (1802-1888) Papers, 1832/18561
- Alfred Leyburn Papers, 1823/1899, bulk 1830/18391
- Alice Rice Jaffe Papers, 1807/1950, bulk 1919/19501
- Allen Family Papers, 1766/19331
- Allen-Johnson Family Papers, 1838/19471
- Allen-Kean-Laurence family letters, 1837/19601
- Alpheus Garrison Civil War Records, 1804/18881
- Alumni Association Records, 1833/2014, bulk 1950/20051
- Alvan Fisher Personal Papers (SC-33), 1822/18521