This is primarily a collection of letters, with some additional documents, concerning Young's interest in botany, geology, mineralogy, and natural history. There is information about Bowdoin College, where he studied under Parker Cleaveland. There is also much on the natural history of Maine, where he was the State Botanist in 1847-1849, and also on the Bangor Natural History Society. There are materials on Brazil in relation to Young's service there as the U.S. consul to Rio Grande do Sul from 1863 to 1873. There are also letters from his brother, John C. Young, and his sister, Sarah Augusta Young.

Letters (including some transcripts and photostats) from and to Vaughan from many American and British correspondents, including: Also personal correspondence and business papers of Benjamin, Charles, Petty, Samuel Sr., Samuel Jr., William, William Oliver, and Sarah Vaughan (2 boxes); lectures, mostly in shorthand (3 vols.); a large number of notes and memoranda on a wide variety of topics, such as agriculture, architecture, astronomy, diplomacy, diseases, dueling, electricity, hieroglyphs, internal improvements, medicine, meteorology, land, manufactures, politics, punctuation, religion, silk-manufacturing, stock-breeding, taxation, Unitarianism, Benjamin Franklin, John Locke, Napoleon I, Joseph Priestley, Bowdoin College, town of Hallowell, Maine; notes on the peace negotiations, 1782-1783; miscellaneous legal papers; genealogy of the Abbott-Vaughan families. For a personal account of the collection, see Mrs. Mary Vaughan Marvin, "The Benjamin Vaughan Papers," APS Proceedings 95 (1951): 246-249.