Per- and poly fluorinated alkyl substances (PFASs), notably perfluorooctanoic acid (PFOA), contaminate many ground and surface waters and are environmentally persistent. The performance limitations of existing remediation methods motivate efforts to develop effective adsorbents. Here we report a β-cyclodextrin (β-CD)-based polymer network with higher affinity for PFOA compared to powdered activated carbon, along with comparable capacity and kinetics. The β-CD polymer reduces PFOA concentrations from 1 μg L-1 to <10 ng L-1, at least 7 times lower than the 2016 U.S. EPA advisory level (70 ng L-1), and was regenerated and reused multiple times by washing with MeOH. The performance of the polymer is unaffected by humic acid, a component of natural organic matter that fouls activated carbons. These results are promising for treating PFOA-contaminated water and demonstrate the versatility of β-CD-based adsorbents.