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. The Coastal Carolinas study area includes the Pee Dee and Cape Fear River Basins and the Atlantic Coastal Plain from Brunswick, Georgia, to near Greenville, North Carolina. The study is divided into 5 main components: 1) Societal Water-Use Data Compilation and Refinement, 2) Land-Use, Population, Water-Use and Climate Change Scenarios, 3) Surface-Water Modeling, 4) Ecological Response Modeling, and 5) Groundwater Modeling. One task to meet this objective was to compile water withdrawal and return data by water-use category from local, regional, and state-scale data sources in order to utilize those data in surface-water models, a groundwater model, an ecological flow model, and for predictions of future water needs. This data release contains (1) Groundwater withdrawals for Georgia, South Carolina, and North Carolina aggregated by groundwater MODFLOW model cell area, year, and water-use category; (2) Surface-water withdrawal estimates for years 1983 - 2017 aggregated to the Soil and Water Assessment (SWAT) model catchment level developed for the Pee Dee and Cape Fear River Basins; (3) Wastewater return estimates from years 2000, 2005, 2010, and 2015 aggregated to the Soil and Water Assessment (SWAT) model catchment level developed for the Pee Dee and Cape Fear River Basins; and (4) Surface-water and groundwater off-stream water-use estimates in the Coastal Carolinas study area for selected water-use categories from years 2000, 2005, 2010, and 2015 aggregated to the 8-digit (subbasin) hydrologic unit level within state boundaries in the Coastal Carolinas study area.