The Payne Harrison Collection consists primarily of manuscripts, notes, and related material for Harrison's novels and other written works (including an unproduced screenplay, Arrow Storm). There is also a considerably large subject file consisting of news articles, government documents, and other materials that Harrison used in research for his works.

Also in the collection are a number of photographs and slides depicting trips Harrison made (to England and to Japan, among other places), as well as various aircraft and other military subjects. (Some photographs are held in the Subject File.)