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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.

Family papers compiled by Katherine Williams of Berkeley Springs, West Virginia. Most of the papers are of the James H. Taylor family of Clarksburg, West Virginia dating from the 19th century. There are also records of the Irwin family including a genealogy, and the Civil War letters of private George Irwin, a soldier in Company F, 95th Ohio Volunteer Infantry. Other families documented include the Redman and Summers families. The collection includes letters, autograph books, family business records, genealogies, photographs, and other material.

Papers of historian, researcher, and author Alan Clarke. He authored a number of books relating to the history of railroads in the region of the state of West Virginia. This collection is minimally processed.

Views of Mount Vernon spanning more than 100 years. The Robert Waldsmith Collection consists of approximately 300 stereographs and cabinet cards by Alexander Gardner, N. G. Johnson, Luke D. Dillon, and others. Highlights of the collection include: several west front views of the Mansion, including the earlist known one by Frederick Langenheim, circa 1856; an early view of the tomb, circa 1857, and a collection of Washington statues and buildings honoring the first President.

The John L. Nau III Civil War History Collection (1806-1988, bulk 1861-1865; 133 cubic feet) contains Civil War-era correspondence, service records, pension records, artifacts, photographs, military records (including orders, requisitions, and correspondence), currency, newspapers, and other print materials.

This collection consists of forty-four nineteenth century photographs, the majority in a carte de viste style, of the Southall, Minor, and Venablefamilies of Charlottesville, Virginia, including two Afro-American family servants.

Papers, chiefly 1847-1887, of James Barron Hope. Correspondence includes letters to his mother Jane A. Barron Hope while on a naval cruise to the Caribbean and letters to his wife, Annie Beverley Whiting Hope written during the Civil War. There are letters between Jane A. Barron Hope and her friend, Caroline Matilda Campbell. Prominent correspondents in the collection include Jubal A. Early, Benjamin S. Ewell, Hugh Blair Grigsby, Fitzhugh Lee, W. H. F. Lee, Thomas Nelson Page, John Tyler and Robert Charles Winthrop. The collection also includes editorials, atories, a play, manuscript poems of Hope including his address at the Yorktown Centennial, as well as articles and letters concerning his death and his involvement in dueling.

Papers, 1770-1875, of the Blow family of "Tower Hill," Sussex County, Va. and of the Waller family. Prominent correspondents in the collection include Philip Barraud, John Hartwell Cocke, Henry Lee and Edmund Ruffin. Most of these accessions were integrated as the collection was partially processed, but some are boxed separately.

Papers, 1800-1901, of and relating to John Hipkins and John Hipkins Bernard (mostly accounts); of and relating to members of the Hipkins, Bernard and Robb families; and relating to the Hipkins-Bernard-Robb home "Rose Hill," Caroline County, Va. (later renamed "Gay Mont") and to Bernard's lands in Alabama, Texas and Arkansas. Includes diaries, correspondence, poems, accounts and account books of women (Elizabeth Hipkins, Jane Gay Robertson Bernard, and Helen Struan Bernard Robb); and legal documents and letters of John Taylor of Caroline. Of special interest are the diaries of Eugenia D. Robb while serving with the American Red Cross in Germany and Japan during and after World War II (1999.56A).