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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.

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 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 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.

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.

Ephemera collected by Geo. Gregory Smart related to the memory and popular image of George Washington. The collection includes postcards, calendars, cigar boxes covers, stamps and first day covers, programs for anniversary events, books and pamphlets, hat stands, billheads, stationary, cartes-de-visite, playing cards, and puzzles. Some items are catchy such as a hat stand touting the motto "friends you can hang your hat on," while others are designed to be more educational such as grade-school primers or the story of the presidents from the makers of Planters peanuts.