- Alexandria Library Records (MS098), 1937/20139
- Alexandria National Bank Collection (MS193), 1904/19781
- Alexandria, Virginia City Records (MS019), 1750/1983, bulk 1825/18751
- Alfonso García Robles papers, 1978/19883
- Alfred A. Bolton, Papers regarding History of Management and Other Material, 1900/200737
- Alfred C. Payne Collection, 1917/200369
- Alice Cartledge Cornett, Journalist, Papers, 1945/2017, bulk 1973/19921
- Alice Huffman Bugel Collection (Eighth Evacuation Unit Hospital), 1942/20001
- Alice Langley Hsieh Papers, 1943/19785
- Alice McMechen, Collector, Papers of Artist Alvena V. Seckar, 1945/20083
- Aliquando Press Collection, 19681
- Allan Blank Papers, 1958/200912
- Alleghany Chapter, National Society of the Daughters of the American Revolution Records, 1890/202222
- Allegheny Highlands Project Records, 1970/198228
- Alliance of Women in Architecture (AWA) Records, 1992/19982