- Early Records of the Mount Vernon Ladies' Association, 1853/1951, bulk 1853/18751
- Financial Records of the Mount Vernon Ladies' Association, 1858/20154
- Geo. Gregory Smart collection of Washington and Mount Vernon ephemera, 1793/20178
- Historic ephemera collection, 1796/19863
- Historic newspapers collection, 1757/19574
- Historical Photograph Collection, 1850/20101
- John Augustine Washington III and family papers, 1789/19944
- Morley Jeffers Williams Collection, 1602/19677
- Papers of the Mount Vernon Ladies' Association, 1858/20164
- Papers of the Superintendent and Resident Director, 1850/19963
- Peter family papers, 1722/19324
- Publications - History of Mount Vernon and George Washington, 1854/20123
- Publications and Printed Material of the Mount Vernon Ladies' Association, 1854/20165
- Restoration Files for the Historic Structures Report, 1750/20052
- Robert Waldsmith Collection of stereographs and cabinet cards, 1856/19811