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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.

Maps collected by, or created by, Mount Vernon staff and the Mount Vernon Ladies' Association. Includes maps of the estate itself, as well as the surrounding neighborhood, the viewshed, and Fairfax County. Dates range from the 1850s to 1992, with bulk dates in the 1930s-1960s.