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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 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 collections contains the architectural drawings of Mount Vernon including the measured drawings of the Mansion, outbuildings, and other MVLA structures. The bulk of material dates from the 1930s (during the tenure of the Director of Research and Restoration, Morley Jeffers Williams) through the 1990s. The drawings were accumulated by, and transferred to, the library/archives over time and are now compiled into this collection based on format and purpose.

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.

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 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.

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 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.

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.

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.