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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.

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.

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.

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.

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.

The collection consists of correspondence, reports, surveys, newspaper clippings, biographies and other written works, bibliographies, excerpts from diaries, letters, inventories and ledgers, various types of architectural and archaeological drawings, maps, and images documenting the work and research conducted during Morley Jeffers Williams's tenure at George Washington's Mount Vernon. Williams compiled the majority of the documents and images found in this collection between 1931 and 1939; however, the information contained within these records dates from 1602 to 1967. The bulk of the collection consists of numerous architectural and archaeological drawings detailing past and contemporary views of George Washington's estate; furthermore, there are several drawings depicting possible future renovations to Mount Vernon. This collection also contains a large amount of scholarly research pertaining to George Washington, Mount Vernon, and 18th-century life and culture. This information provides an in-depth understanding of George Washington's life, particularly concerning his interactions with his estate. Other documentation charts the efforts of Morley Jeffers Williams as he worked to restore the structures and landscape at Mount Vernon.

Educating the public on the life and legacy of George Washington, colonial life, slavery, and other relevant subjects is part of the MVLA's mission. The publication of books, brochures, and other printed material is one aspect of achieving this goal. This collection combines all printed formats published by the Mount Vernon Ladies' Associaton including books, booklets, brochures, information sheets, event announcements, bylaws, and handbooks or guidebooks. Annual Reports and the Minutes of the Council provide background and information on the yearly activities and business of the Mount Vernon Ladies' Association. The material includes a wide date range, 1854 to the present.

This collection contains publications concerning the history of Mount Vernon and George Washington that were not published by the Mount Vernon Ladies' Association. The MVLA collaborated with other authors and publishers to produce many of these titles, however the Association was not the copyright holder. These items have been merged together into this collection but are from different sources or accessions. Most of the publications were either originally collected by the Library at Mount Vernon, or were previously owned by Vice Regents of the Association. Others were given as gifts to the MVLA.

This collection includes bound volumes of primary sources by the Superintendent or Resident Director of Mount Vernon: the letter books and diaries of Superintendent Harrison H. Dodge from the 1885 to 1927, and the monthly reports to the Regent by Superintendent (later Resident Director) Charles Cecil Wall for the years 1948-1967. Dodge's letter books contain letterpress and handwritten copies of outgoing correspondence. These were bound into 32 volumes in 1968-1969. The majority of these letters are to the Regent, and some take the form of a monthly report. Dodge's diaries include handwritten day-to-day descriptions of the activities going on at Mount Vernon. Copies of Mr. Wall's monthly reports to the Regent were also bound in 1968 "for ready reference." (Council Minutes 1968) The monthly reports and some of Dodge's correspondence are also found in the Papers of the Superintendent and Resident Director.