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The Historical Photograph Collection is largely comprised of materials created by or for the Mount Vernon Ladies' Association. Some of the earliest photographs of the estate were created and sold to visitors by the Association as a means of income. Those efforts helped to establish an important collection of 19th century views. The collection spans the 1850s to 2000s and includes over 140 linear feet of analog material providing a visual history of the Mansion, outbuildings, tombs, grounds, events, visitors, collection objects, personnel, and changes throughout the estate.

The oral histories collected by the MVLA and the Washington Library include personal memories and reminiscences of previous Regents, Vice Regents, and Mount Vernon employees. Much of the collection was recorded during the 2000s-2010s by staff members Sandra Robinette and Mary Thompson. This collection grows and accrues more recordings every year as other long-term employees and Board members contribute their stories. Mount Vernon's oral histories were often recorded via audio tape, some of which were then transferred to CD. The most recent interviews were digitally recorded and are only accessible in that format, or via the transcriptions. The date range of this collection is 1983-2021, but it is consistently updated.