The vocabularies comprising the American Indian Vocabulary Collection were assembled by the Historical and Literary Committee in 1816, when preparing for the first volume of their Transactions. The resulting collection consists of 23 vocabularies of 19 languages collected between 1784 to 1828, along with letters of transmittal and other associated information. A number of individuals were invovled in recording the vocabularies, including Benjamin Hawkins, William Thornton, David Campbell, Daniel Smith, Constantine Volney, Constantine Rafinesque, William Vans Murray, John Heckewelder, Martin Duralde, Campanius Holm, and Jefferson himself.

The majority of the vocabularies record languages in what is now the eastern half of the United States, ranging from Osage, Quapaw, and Shawnee in the lower Mississippi Valley to Natick and Mohegan in New England. Rafinesque submitted vocabularies for two non-North American languages, the extinct Taino language of Haiti and for Chontal in Central America, and Jefferson himself recorded one vocabulary, Unquachog from the Pusspatock settlement near Brookhaven, Long Island.

A number of the original printed forms of the Jefferson vocabulary (ca. 1790-1792) are included. These materials were in many instances copied by Peter S. Du Ponceau into his private collection of Indian vocabularies (Mss. 497 In2) and were, in this form, utilized by Albert Gallatin for his Synopsis (1836). Gallatin had also seen the Jefferson manuscripts.