The Pee Dee and Cape Fear River Basins in North Carolina and South Carolina were chosen as a focus area study (FAS) for the U.S. Geological Survey (USGS) National Water Census (NWC) in 2016. The objective of the NWC is to place technical information and tools in the hands of stake holders so that they can make decisions on water availability. The USGS South Atlantic Water Science Center, comprised of North Carolina, South Carolina, and Georgia, conducted a 3-year study of water use and availability to provide information related to the competing societal and ecological water needs in the Southeastern Atlantic Coastal Basins of the Carolinas. One task to meet this objective was compiling water withdrawal and return data by category from local, regional, and state-scale data sources so that those data could be utilized in surface-water models, a groundwater model, an ecological flow model, and for predictions of future water needs. This dataset presents wastewater-return estimates from years 2000, 2005, 2010, and 2015 which are aggregated to the Soil and Water Assessment Tool (SWAT) model catchment-area level developed for the Pee Dee and Cape Fear River Basins.