- Anniversaries and Commemorations Collection, 1981/20001
- Audio Visual Collection, 1928/20152
- Financial Records of the Mount Vernon Ladies' Association, 1858/20158
- Geo. Gregory Smart collection of Washington and Mount Vernon ephemera, 1793/20175
- Historic ephemera collection, 1796/19862
- John Augustine Washington III and family papers, 1789/19941
- Papers of Christine Meadows, Curator, 1960/19975
- Papers of Mary V. Thompson, Research Historian, 1980/20122
- Papers of the Mount Vernon Ladies' Association, 1858/20169
- Papers of the Superintendent and Resident Director, 1850/19964
- Publications - History of Mount Vernon and George Washington, 1854/20124
- Publications Committee Collection, 1951/19972
- Publications and Printed Material of the Mount Vernon Ladies' Association, 1854/20166
- Restoration Files for the Historic Structures Report, 1750/20053
- Robert Waldsmith Collection of stereographs and cabinet cards, 1856/19811