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The Historical Photograph Collection is largely comprised of materials created by or for the Mount Vernon Ladies' Association. Photographers primarily include staff members and contract photographers. The collection spans the 1930s to the 2000s and includes analog material made up of a variety of sizes of film negatives providing a visual history of the Mansion, outbuildings, tombs, grounds, events, visitors, collection objects, personnel, restoration, and changes throughout the estate.

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 Historical Photograph Collection is largely comprised of materials created by or for the Mount Vernon Ladies' Association. Some of the earliest photographs of the estate were created and sold to visitors by the Association as a means of income. Those efforts helped to establish an important collection of 19th century views. The collection spans the 1850s to 2000s and includes over 140 linear feet of analog material providing a visual history of the Mansion, outbuildings, tombs, grounds, events, visitors, collection objects, personnel, and changes throughout the estate.

This collection combines the papers and files of each Superintendent or Resident Director listed under "Creators," as well as their office staff, assistants, and other Mount Vernon personnel. The bulk of this collection consists of correspondence to and from each Superintendent or Resident Director. Other types of material include reports, essays, memos, publications, clippings, official forms, logs or diaries of events, calendars, schedules, photographs, and ephemera. Subject matter includes a wide variety of topics and concerns for operating and maintaining an historic house. The Resident Directors oversaw almost all major projects and events around Mount Vernon such as building and grounds maintenance, restoration, fundraising, collection of historic artifacts, visitor engagement, and administrative functions. Dodge and Wall were both well known for their involvement in even the smallest details of the operation of Mount Vernon and this is reflected in the volume and scope of their files. Later Resident Directors began keeping chronological files which are also a great resource for understanding projects from specific years and periods of Mount Vernon's history. Both Charles Wall and John Castellani were employees of Mount Vernon before they were appointed Resident Director, and their files include material from previous job assignments. The majority of material reflects Charles Wall's tenure as Resident Director, the 1930s to 1970s, however, there is a substantial amount from the other directors as well. Several folders may extend into the term of James (Jim) Rees who served as Resident Director (later President) of Mount Vernon from 1994 to 2012. Most of the letters written by Superintendent Harrison Dodge were laminated or adhered to a tissue or paper backing, and bound together into a multiple volume set. These bound volumes, along with the original work diaries kept by Dodge, have been combined into a separate collection, the Bound Volumes of Superintendent's Letters, Diaries, and Monthly Reports. A finding aid for this collection is also available.

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 includes ephemera from 1796-1986, and contains a variety of formats that primarily relate to the portrayal of George Washington.

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 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.