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The nucleus of this collection was created from papers given to the Association by Ann Pamela Cunningham around the time of her retirement as Regent. Several other Vice Regents followed her example and later donated their papers as well. These records were referred to as the "Early Records" since the time they were first established as an archival collection. A large portion of this collection is correspondence concerning the founding of the MVLA and the operation of Mount Vernon as a historic site. Other important resources are the appeals written by Ann Pamela Cunningham and the Vice Regents, governing documents, subscription or donation lists, printed material or publications, and bound volumes such as ledgers or scrapbooks. Individual items were added to the collection as they were acquired. The Early Records includes items dated 1852-1951, however the bulk of the material dates from 1858 to around 1880.

This collection holds the historic financial records of the MVLA including accounting ledgers, tax documents, insurance papers, receipts, invoices, payroll lists, annual and quarterly budgets, financial statements and reports, policies, contracts, correspondence, and other miscellaneous items. Records in this collection contain information on the Association's financial accounting, revenue, expenditures, employees and employee benefits, investments, taxes, and other financial concerns. There is a very limited amount pertaining to fundraising efforts and/or private donations, which can be found in the files of Mount Vernon's development department (currently unprocessed). Bulk date 1870s-2000s.

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.

Views of Mount Vernon spanning more than 100 years. The Robert Waldsmith Collection consists of approximately 300 stereographs and cabinet cards by Alexander Gardner, N. G. Johnson, Luke D. Dillon, and others. Highlights of the collection include: several west front views of the Mansion, including the earlist known one by Frederick Langenheim, circa 1856; an early view of the tomb, circa 1857, and a collection of Washington statues and buildings honoring the first President.