The production of nuclear materials for the national defense was an intense, nationwide effort that began with the Manhattan Project and continued throughout the Cold War. Now many of these product materials, by-products, and precursors, such as irradiated nuclear fuels and targets, have been declared as excess by the Department of Energy (DOE). Most of this excess inventory has been, or will be, turned over to DOE's Office of Environmental Management (EM), which is responsible for cleaning up the former production sites. Recognizing the scientific and technical challenges facing EM, Congress in 1995 established the EM Science Program (EMSP) to develop and fund directed, long-term research that could substantially enhance the knowledge base available for new cleanup technologies and decision making. The EMSP has previously asked the National Academies' National Research Council for advice for developing research agendas in subsurface contamination, facility deactivation and decommissioning, high-level waste, and mixed and transuranic waste. For this study the committee was tasked to provide recommendations for a research agenda to improve the scientific basis for DOE's management of its high-cost, high-volume, or high-risk excess nuclear materials and spent nuclear fuels. To address its task, the committee focused its attention on DOE's excess plutonium-239, spent nuclear fuels, cesium-137 and strontium-90 capsules, depleted uranium, and higher actinide isotopes.