The confluence of pervasiveness, bioaccumulation, and toxicity in freshwater contaminants presents an environmental threat second to none. Exemplifying this trifecta, per- and polyfluoroalkyl substances (PFAS) present an alarming hazard among the emerging contaminants. State-of-the-art PFAS adsorbents used in drinking water treatment, namely, activated carbons and ion-exchange resins, are handicapped by low adsorption capacity, competitive adsorption, and/or slow kinetics. To overcome these shortcomings, metal–organic frameworks (MOFs) with tailored pore size, surface, and pore chemistry are promising alternatives. Thanks to the compositional modularity of MOFs and polymer–MOF composites, herein we report on a series of water-stable zirconium carboxylate MOFs and their low-cost polymer-grafted composites as C8–PFAS adsorbents with benchmark kinetics and “parts per billion” removal efficiencies. Bespoke insights into the structure–function relationships of PFAS adsorbents are obtained by leveraging interfacial design principles on solid sorbents, creating a synergy between the extrinsic particle surfaces and intrinsic molecular building blocks.