The U.S. Geological Survey Groundwater Ambient Monitoring and Assessment-Priority Basin Project (USGS GAMA-PBP) collected samples to be analyzed for per-and polyfluoroalkyl substances (PFAS) from domestic and public supply wells from May 2019 to September 2020. The datasets presented here include identification of the 28 PFAS constituents monitored by the project, Identification and brief characterization of the 211 GAMA-PBP wells for which samples were analyzed for PFAS during the study period, and analytical results for those groundwater samples, along with results for quality control samples.