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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 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 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.

This collection consists of papers collected by various members of the Peter families. It includes letters from George Washington, letters of condolence to Martha Washington after George Washington's death, estate documents, Major George Peter's military papers, land plats and surveys, photo albums, letterbooks, and notebooks that tell of the life of this prominent family in Virginia and the City of Washington.

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.