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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.

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.

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 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 holds the historic financial records of the MVLA including accounting ledgers, tax documents, insurance papers, receipts, invoices, payroll lists, annual and quarterly budgets, financial statements and reports, policies, contracts, correspondence, and other miscellaneous items. Records in this collection contain information on the Association's financial accounting, revenue, expenditures, employees and employee benefits, investments, taxes, and other financial concerns. There is a very limited amount pertaining to fundraising efforts and/or private donations, which can be found in the files of Mount Vernon's development department (currently unprocessed). Bulk date 1870s-2000s.

The Papers of Harrison H. Dodge is a small collection of material created and compiled by Dodge and/or his family. Types of records include correspondence, articles, family trees, news clippings, photographs, and several objects. Most of the items pertain to Dodge's time as Superintendent at Mount Vernon, however there are some personal family letters, genealogy information, and items regarding his work on a Library of Congress committee. Some genealogical records, mostly fragments and scraps of paper, may date as early as the 1770s, however the bulk of material in the collection dates from the 1880s to the 1930s. The earliest dated item in the collection is a Dodge family bible, c. 1816.

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.

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 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.

Maps collected by, or created by, Mount Vernon staff and the Mount Vernon Ladies' Association. Includes maps of the estate itself, as well as the surrounding neighborhood, the viewshed, and Fairfax County. Dates range from the 1850s to 1992, with bulk dates in the 1930s-1960s.