Total fine particle mass (pm25), organic carbon fine particle mass (oc), sulfate fine particle mass (so4), and sulfur dioxide gas (so2) observed EPA AQS sites (ob) and predicted by the CMAQ-CRACMM model v5.4 (mod) for summer 2019 in the United States used in the study of Vannucci et al. ACS ESC 2024. Additional data includes AQS site identifiers as well as ambient air temperature. Aerosol concentrations are in micrograms per cubic meter of air (ug/m3), temperature is in degrees Celsius (iC), and sulfur dioxide is in parts per billion by volume (ppb). Links are provided to obtain the CMAQ code and raw AQS observations.