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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.

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 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 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.

Materials relating to the career of Lester Jesse Cappon (September 18, 1900-August 24, 1981), historian and formerly the Archivist for the Colonial Williamsburg Foundation, Williamsburg, Virginia, Director of the Institute of Early American History and Culture, and Senior Research Fellow at the Newberry Library, Chicago, Illinois.