- Audio Visual Collection, 1928/20151
- Early Records of the Mount Vernon Ladies' Association, 1853/1951, bulk 1853/18751
- Financial Records of the Mount Vernon Ladies' Association, 1858/20155
- Geo. Gregory Smart collection of Washington and Mount Vernon ephemera, 1793/201710
- Historic ephemera collection, 1796/19865
- Historic newspapers collection, 1757/19575
- Historical Photograph Collection, 1850/20101
- John Augustine Washington III and family papers, 1789/19943
- Morley Jeffers Williams Collection, 1602/19676
- Papers of the Mount Vernon Ladies' Association, 1858/20167
- Papers of the Superintendent and Resident Director, 1850/19964
- Peter family papers, 1722/19322
- Publications - History of Mount Vernon and George Washington, 1854/20124
- Publications and Printed Material of the Mount Vernon Ladies' Association, 1854/20166
- Restoration Files for the Historic Structures Report, 1750/20052