The voluminous Anthony Wallace Papers contain a wealth of material for scholars of anthropology, history, and psychiatry. At first glance, the collection appears quite eclectic, yet common themes of technological, social, and cultural change unite the seemingly disparate subjects, providing a broad range of source materials for the study of technological and social change, American Indians, personality and culture, revitalization movements, the cultural and biological bases of behavior, and Pennsylvania history, particularly that of Delaware and Schuylkill Counties.

Along with Wallace's correspondence to and from such anthropologists as Frank G. Speck, A. Irving Hallowell, William N. Fenton, Floyd Lounsbury, and others, the collection includes extensive correspondence with knowledgeable local historians, reflecting Wallace's awareness of the benefits as well as the liabilities of their homegrown knowledge. There is extensive correspondence from Merle Deardorff of Warren, Pennsylvania and Robert Scherr of Schuylkill County; Deardorff's correspondence in particular provides a wealth of information on Iroquois history and traditions as well as the occasional sharp and uncompromising criticism of Wallace's work.

Wallace's research notes, drafts of his works, and photocopies of primary source material from various repositories and reprints of secondary sources comprise the majority of the collection. His assemblage of 19th century census and tax records, church records, and local histories for the Pennsylvania towns of Rockdale and St. Clair provides researchers with a centralized resource of materials from various repositories. Card files of information collected on various families of Delaware and Schuylkill Counties represent a valuable resource for scholars of Pennsylvania history as well as genealogists. The reprints, on topics ranging from social and technological change, personality and culture, and psychiatric research to Indian history and Pennsylvania coal region history appear in the subseries related to these subjects.

News clippings and magazine articles related to Wallace's work appear throughout the collection. The most significant include articles on federal efforts to recruit anthropologists for counterinsurgency and other politically-motivated missions, particularly in Thailand, and the Kinzua Dam controversy, when the state of New York built a dam that flooded much of the historic Cornplanter Grant on the Allegany Reservation. The collection also contains extensive materials on the Indian land claims cases of the 1950s, in which Wallace served as an expert witness.

Notes and research materials for Wallace's works since 1990 are not currently included in the collection, but Series IV, Works by Wallace, does include the original manuscript draft of his 1999 work on Thomas Jefferson and the Indians under the working title Logan's Mourner.

In addition to documenting the Wallaces' professional careers, the collection documents the personal side of their family through correspondence, photograph albums, and histories dating from the 1920s that also describe 19th century people and events. The family albums include three histories compiled by Paul A.W. Wallace; two histories compiled by Paul Wallace's father, clergyman Francis Huston Wallace; 19th century images of Wallace ancestors, homes, and the Wallace family library; photographs of Anthony Wallace and his brother David from childhood through adulthood; and Anthony Wallace's World War II scrapbook of photographs from his military service, which includes original photographs of Germany in 1945. The collection also includes Anthony Wallace's scrapbooks and notebooks as well as his writings from childhood through adolescence.