Per- and polyfluoroalkyl substances (PFAS) are persistent contaminants of increasing global concern. However, the efficient removal of short-chain PFAS from highly contaminated sources is largely inefficient, and the management of regenerated PFAS streams remains challenging. In this study, we report the design and preparation of a series of efficient and regenerable ion-exchange resin beads that can be directly employed in a continuous cartridge setting for efficient short-chain PFAS removal from landfill leachate. The beads consist of a crosslinked polystyrenic network bearing covalently attached selective sorption segments and permanently charged quaternary ammonium groups. The spherical morphology of beads minimizes swelling induced pressure buildup in packed bed configurations, enabling long-term and stable PFAS treatment. Batch experiments show >90% PFAS removal over five regeneration cycles, while rapid small-scale column tests demonstrate a >10,000-fold increase in breakthrough bed volumes compared with the commercial resin PFA694E. The concentrated PFAS eluate generated during regeneration is subsequently employed as an electrolyte additive for aqueous zinc batteries, where the fluorinated species are destructed into a ZnF2-rich interphase. As a result, both symmetric and full cells exhibit enhanced cycling stability and improved capacity retention compared with additive-free control batteries. This pathway converts PFAS from a contaminant into a useful electrochemical material, supporting sustainable water treatment and resource recovery.