- Financial Records of the Mount Vernon Ladies' Association, 1858/20154
- Geo. Gregory Smart collection of Washington and Mount Vernon ephemera, 1793/20172
- Guest Books and Visitor Registers, 1850/20161
- Historical Photograph Collection, 1850/201079
- John Augustine Washington III and family papers, 1789/19942
- Lawrence Washington collection of Washington family papers, 1787/19321
- Mount Vernon and MVLA Ephemera, 1858/20221
- Papers of the Mount Vernon Ladies' Association, 1858/20162
- Papers of the Superintendent and Resident Director, 1850/19961
- Peter family papers, 1722/19321
- Publications - History of Mount Vernon and George Washington, 1854/20123
- Publications and Printed Material of the Mount Vernon Ladies' Association, 1854/20161
- Restoration Files for the Historic Structures Report, 1750/20051
- Robert Waldsmith Collection of stereographs and cabinet cards, 1856/19814
- Superintendent's Letter Books, Diaries, and Monthly Reports - collection of bound volumes, 1885/19673