The Correspondence series contains items sent and received by Coale over the course of his career at Princeton. The series has two divisions: Chronological (1954-1998) and Topical (1954-1998). Chronological is often outgoing correspondence, though both contain a variety of letters to and from other demographers in Princeton, the United States, and abroad. Many provide details regarding the scope and progress of Coale's research projects. Others relate to travel and his participation in professional organizations, particularly the International Union for the Scientific Study of Population (IUSSP). A large amount of correspondence is between Coale and Edgar M. Hoover, with whom he authored the Coale-Hoover report.

The Papers and Projects series is a compilation of Coale's writings, including texts of lectures, reprints of published manuscripts, data, correspondence, and other articles collected by Coale during his research. Notable projects include demographic studies conducted about India (1950s), Mexico (1950s and 1970s), China (1970s and 1990s), and the countries of the former Soviet Union (1990s).