Data from a laboratory study undertaken at the U.S. Geological Survey to investigate solid/water partitioning of per- and polyfluoroalkyl substances (PFAS) in New Hampshire soils and biosolids are presented here. Soils and biosolids used for the experiments were collected using PFAS-free sampling equipment, air dried, gently homogenized, and sieved (soils only). Soil samples were collected from locations with known PFAS contamination (n = 5) and nearby sites with similar soil characteristics but low expected PFAS concentrations (n = 4). Finished biosolids were collected directly from facilities at the final stage of processing and before distribution. Air-dried soils and biosolids were then used for a series of batch and column experiments to determine water/solid distribution coefficient (Kd) values. This study investigated the impact of pH, ionic strength, adsorption versus desorption, soil/biosolid type, experimental setup (batch versus column), and influence of sodium azide on Kd values. All batch and column experiments were run for 10 days as determined by a 16-day kinetics test. The dataset presented here includes concentration of PFAS, concentration of PFAS post total oxidizable precursor assay (TOPA), pH, moisture content, total organic carbon concentrations, aluminum concentrations, iron concentrations, sodium concentrations, cation exchange capacity, anion exchange capacity, grain size, and protein concentrations for the unprocessed soil and biosolids collected from the site (soils) or facility (biosolids). These are denoted as "Environmental - Biosolid" or "Environmental - Soil" samples in the data release. The dataset also includes the solid and water results (PFAS, TOPA, pH, specific conductivity, dissolved organic carbon, major anions, and metals) from the batch and column experiments, along with the calculated Kd values. Calculated Kd values are presented for every PFAS compound with detections in the solid and water phases and, with caution, can be used to help constrain estimates for PFAS mobility in the New Hampshire environment.