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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 bulk of this collection is made up of letters from Jane Charlotte Washington to her son, John Augustine Washington III. Also included are letters to Eleanor Love Selden Washington, a few letters to or from John Augustine Washington III to various individuals, several letters from George Mason of Hollin Hall (1797-1870) to John Augustine Washington III, letters by Lackland and Alexander family members (relatives of the Washingtons) and three receipts. The subject matter of most letters is family or personal affairs and Mount Vernon business with some discussion of the enslaved people owned by the Washingtons. Inclusive dates are 1837 to 1861.

The collection contains correspondence between John Augustine Washington III and his wife Eleanor Love Selden. The letters begin during the Washingtons' engagement and continues through eighteen years of marriage, ending with a letter from John Augustine to Eleanor composed the day prior to her sudden death. The letters contain information on family matters, the management of the Mount Vernon estate, and plantation life prior to the Civil War.

This collection contains correspondence, legal documents, financial records, and other documents related to John Augustine Washington III and his family, especially his son, Lawrence, as well as his granddaughters, Anne and Patty. The bulk of the correspondence series are letters sent to John Augustine Washington III and concern family affairs and the management of various family plantations, including Mount Vernon.

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.

A large portion of this collection consists of letters to and from John Augustine Washington III related to the sale of Mount Vernon. Other items include family wills, legal documents, receipts, correspondence related to Washington relics, as well as several photographs and miscellany. Inclusive dates, 1787-1932.