On account of its nonbiodegradable nature and persistence in the environment, perfluorooctanoic acid (PFOA) accumulates in water resources and poses serious environmental issues in many parts of the world. Here, we present the development of two fluorine-rich calixarene-based porous polymers, FCX4-P and FCX4-BP, and demonstrate their utility for the efficient removal of PFOA from water. These materials featured Brunauer-Emmett-Teller (BET) surface areas of up to 450 m2 g-1, which is slightly lower than their nonfluorinated counterparts (up to 596 m2 g-1). FCX4-P removes PFOA at environmentally relevant concentrations with a high rate constant of 3.80 g mg-1 h-1 and reached an exceptional maximum PFOA uptake capacity of 188.7 mg g-1. In addition, it could be regenerated by simple methanol wash and reused without a significant decrease in performance.