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Per- and polyfluoroalkyl substances (PFAS) are man-made environmental contaminants causing increasing global concern due to their adverse effect on environmental and human health. Conventional treatment methods are ineffective in removing short-chain PFAS because they are persistent and recalcitrant to treatment. This study evaluated the performance of a structurally-tunable and chemically-stable porous organic polymer (POP) for PFAS removal under realistic environmental conditions. The POP demonstrated an exceptionally high removal efficiency (>95%) within 15 min when the initial PFAS concentration was approximately 400 ng/L. The adsorption of PFAS on the POP was not significantly affected by changes in solution pH within the range of 5–9. The common co-contaminants in water competed with short-chain PFAS for active sites during the adsorption process following the order of natural organic matter (NOM), long-chain PFAS, and Cl−. The Freundlich-type model could predict the multicomponent interactions well with a R2 value above 0.91. The spent POP was effectively regenerated using a mixture of the 10% NaCl and 30% methanol solution and the PFAS removal maintained at 90% through five adsorption and desorption cycles. The characteristics of the designed POP make it a highly promising and stable absorbent. It enables fast and effective removal of short-chain PFAS. [Display omitted] • Cationic POP shows a fast adsorption rate and a high capacity for PFAS removal. • The designed POP maintained above 85% removal for PFBA at a pH range of 5–9. • The effect of the co-contaminants on PFBA removal followed the order of HA > PFOS > Cl−. • PFAS removal maintained at 90% in five consecutive adsorption/regeneration cycles. [ABSTRACT FROM AUTHOR]