- Early Records of the Mount Vernon Ladies' Association, 1853/1951, bulk 1853/18754
- Esther Maria Lewis Chapin collection of Washington family documents, 1743/18521
- Financial Records of the Mount Vernon Ladies' Association, 1858/20155
- Geo. Gregory Smart collection of Washington and Mount Vernon ephemera, 1793/20172
- Guest Books and Visitor Registers, 1850/20161
- Harrison H. Dodge Papers, 1816/19361
- Historic manuscript collection, 1601/19333
- Historic newspapers collection, 1757/19573
- Historical Photograph Collection, 1850/201086
- John Augustine Washington III and family papers, 1789/19944
- Mount Vernon Black and White Film Collection, 1933/200516
- Mount Vernon and MVLA Ephemera, 1858/20222
- Papers of the Mount Vernon Ladies' Association, 1858/20164
- Peter family papers, 1722/19323
- Publications and Printed Material of the Mount Vernon Ladies' Association, 1854/20161