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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.

This collection documents the care and management of Mount Vernon through the work of the MVLA. Types of material include correspondence, reports, memos, notes, personal and biographical information, news clippings, meeting agendas, photographs, scrapbooks, and ephemera. Several highlights of the collection include the original minutes of Council meetings, scrapbooks and ledgers created by Vice Regents, and early correspondence with Regents and Vice Regents. While the library's collection "Early Records of the MVLA" documents the founding and early years of the organization, the Papers of the MVLA continues where that collection ended and preserves the ongoing story of these women and the fulfillment of their mission. Creators of the collection are largely the board members themselves, along with staff and employees who worked directly with them. Scope notes have been added before the content list of each series to better describe its specific provenance and content. The bulk of the collection dates from the 1950s to the 1990s, however there is a very wide range represented overall, 1858-2016.