Per- and polyfluorinated alkyl substances (PFASs) contaminate groundwater, surface water, and finished drinking water internationally. Their ecological persistence and adverse human health effects demand effective remediation approaches. Motivated by the limitations in selectivity and performance of current PFAS removal technologies, we report a platform approach for the development of ionic fluorogel resins that effectively remove a chemically diverse mixture of PFAS from water. The synthesis of a material library with systematic variation in fluorous and ionic components led to the identification of a resin that demonstrated rapid removal of PFASs with high affinity and selectivity in the presence of nonfluorous contaminants commonly found in groundwater. The material can be regenerated and reused multiple times. We demonstrate ionic fluorogels as effective adsorbents for the removal of 21 legacy and emerging PFASs from settled water collected at the Sweeney Water Treatment Plant in Wilmington, North Carolina.