). MOF-818 also exhibits excellent selectivity against common coexisting ions and retains 97% of its capacity after eight regeneration cycles. Combined experimental and computational analyses confirm that chemisorption at OMSs initiates the process and enables subsequent physisorption. This work highlights the power of engineering dual adsorption modes within a single MOF platform as a superior strategy for rapid and high-capacity remediation of per- and polyfluoroalkyl substances (PFAS).