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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.

The Bushrod Washington Family Papers consist of documents gathered by the descendants of the first President of the United States, George Washington. The collection comprises an assortment of correspondence and legal documents documenting the lives and property ownership of several branches of the Washington family. The collection is organized into five series: Correspondence, Legal Documents, Social, Miscellaneous, and Indenture Notices (Land Deeds).

The bulk of this collection is correspondence to Mrs. Laughton concerning Mount Vernon and the work of the Mount Vernon Ladies' Association. Other material includes correspondence from Mrs. Laughton, formal reports and papers of the MVLA, personal correspondence and memoirs, photographs, printed material, and ephemera. The overall dates range from 1850 to 1891 with the bulk of the collection dating from the 1860s-1880s.

This collection concerns the inheritance, maintenance, and sale of the Mount Vernon estate by its last private owner, John Augustine Washington III. A large majority of the collection is correspondence to or from John Augustine Washington III with a significant portion relating to the purchase of the estate by the Mount Vernon Ladies' Association. Three diaries kept by John Augustine are also included and contain important information about his slaves, agricultural practices, and finances. Other types of material in the collection include legal documents, receipts, photographs, and ephemera. Photocopies were made for most of the manuscripts and can be viewed as surrogates to the originals.

This collection of historic manuscripts dates from 1607-1933, with the bulk of materials dating from 1738-1868. The correspondence, journals and diaries, legal and financial records, estate documents, and printed ephemera in the collection primarily relate to the Washington and Custis families, the Revolutionary War, and society life in antebellum Washington D.C. and Virginia.

Educating the public on the life and legacy of George Washington, colonial life, slavery, and other relevant subjects is part of the MVLA's mission. The publication of books, brochures, and other printed material is one aspect of achieving this goal. This collection combines all printed formats published by the Mount Vernon Ladies' Associaton including books, booklets, brochures, information sheets, event announcements, bylaws, and handbooks or guidebooks. Annual Reports and the Minutes of the Council provide background and information on the yearly activities and business of the Mount Vernon Ladies' Association. The material includes a wide date range, 1854 to the present.

This collection contains publications concerning the history of Mount Vernon and George Washington that were not published by the Mount Vernon Ladies' Association. The MVLA collaborated with other authors and publishers to produce many of these titles, however the Association was not the copyright holder. These items have been merged together into this collection but are from different sources or accessions. Most of the publications were either originally collected by the Library at Mount Vernon, or were previously owned by Vice Regents of the Association. Others were given as gifts to the MVLA.