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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.

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.