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Correspondence, manuscripts, notes, notebooks, documents, photographs, course-related materials, and printed materials. The manuscripts include typescripts of Sykes' published and unpublished novels, monographs, plays, short stories, and articles. Among these are The Perennial Avant Garde, The Cool Millennium, and The Hidden Remnant. Sykes' notes and notebooks span the period from the early 1930s to 1980, and include preliminary ideas and sketches for his books, as well as autobiographical material. A small number of documents concern Sykes' wartime work in the U.S. Government Office of War Information. Course-related material including writings and correspondence of students taught by Sykes between 1962 and 1975 at the New School and as an adjunct professor at Columbia University. Printed materials consist of numerous reviews of Sykes' books, in addition to offprints and articles by Sykes. Included as well are printed materials about or connected with Sykes, offprints of articles inscribed to him, and many volumes from his library. The substantial correspondence series includes personal letters and correspondence with agents and publishers relating to his books. Correspondents include Harold Clurman, Aaron Copland, Lawrence Durrell, Georgia O'Keeffe, and Francis Steegmuller, as well as a number of Sykes' students. There is extensive correspondence between Sykes and the artist John Hartell from 1927 to 1983.

Correspondence, playscripts, screenplays, scenarios, short stories, and other manuscripts, drafts, photocopies, contracts and other documents, tearsheets, clippings, and other materials relating to his career as a screenwriter, playwright, and author of short stories. Correspondence with friends, students, admirers, and professional colleagues concern his teaching, playwriting, films, articles, photography, and literary topics. There are also two groups of letters from students and readers about his textbook, "The Human Nature of Playwriting" (1949). Among the cataloged correspondence are William Gibson, MacKinlay Kantor, Anna Louise Strong, Louis Untermeyer, and Carl Van Doren. Included are manuscripts, drafts, or photocopies of almost all his films, plays, and short stories, such as playscripts and drafts of his plays, "The Jazz Singer" (1922), "Skylark" (1939), "Jason" (1942), and others; screenplays and scenarios, many in photocopy, of "Trouble in Paradise" (1932), "The Merry Widow" (1934), "The Shop Aroung the Corner" (1940), "Suspicion" (1941), "Heaven Can Wait" (1943), and many other films; and manuscripts, drafts, tearsheets, and printed copies of his short stories and articles of film and television criticism. There are also many clippings and reviews, programs, and other printed materials about his plays and films.