The Cape Fear and Pee Dee 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 water-use category from local, regional, and state-scale data sources and utilizing those data in Surface-water models, a Groundwater model, an Ecological flow model, and for predictions of future water needs. This data release presents surface-water withdrawals for the Pee Dee and Cape Fear HUC4 river basins in North and South Carolina.