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The widespread production and use of multi-fluorinated carbon-based substances for a variety of purposes has contributed to the contamination of the global water supply in recent decades. Conventional wastewater treatment can reduce contaminants to acceptable levels, but the concentrated retentate stream is still a burden to the environment. A selective anion-exchange membrane capable of capture and controlled release could further concentrate necessary contaminants, making their eventual degradation or long-term storage easier. To this end, commercial microfiltration membranes were modified using pore functionalization to incorporate an anion-exchange moiety within the membrane matrix. This functionalization was performed with primary and quaternary amine-containing polymer networks ranging from weak to strong basic residues. Membrane loading ranged from 0.22 to 0.85 mmol/g membrane and 0.97 to 3.4 mmol/g membrane for quaternary and primary functionalization, respectively. Modified membranes exhibited a range of water permeances within approximately 45–131 LMH/bar. The removal of PFASs from aqueous streams was analyzed for both “long-chain” and “short-chain” analytes, perfluorooctanoic acid and perfluorobutyric acid, respectively. Synthesized membranes demonstrated as high as 90% rejection of perfluorooctanoic acid and 50–80% rejection of perfluorobutyric acid after 30% permeate recovery. Regenerated membranes maintained the capture performance for three cycles of continuous operation. The efficiency of capture and reuse can be improved through the consideration of charge density, water flux, and influent contaminant concentration. This process is not limited by the substrate and, thus, is able to be implemented on other platforms. This research advances a versatile membrane platform for environmentally relevant applications that seek to help increase the global availability of safe drinking water.