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This study evaluated optimal locations for in situ remediation of per‐ and poly‐fluoroalkyl substances (PFAS) in groundwater with colloidal activated carbon (CAC). New Freundlich isotherms for PFAS adsorption to CAC were estimated to illustrate the effect of competitive adsorption with dissolved organic carbon and other PFAS in a groundwater sample. A hypothetical model scenario was constructed based on source area characteristics similar to a site impacted by aqueous film forming foam in South Dakota. Modeling indicates that, even with high PFAS concentrations, CAC would still be capable of maintaining concentrations below proposed maximum contaminant levels in the adsorption zone for at least 30–40 years. Two‐dimensional areal modeling indicates that the future breakthrough of PFAS is likely to occur in the localized core of the plume, and that the corresponding future reinjection of CAC will only need to be conducted over a smaller portion of the original injection footprint. The benefits of implementing a phased remedial approach at PFAS sites are discussed. Source area and mid‐plume CAC treatments are shown to be ineffective at attenuating PFAS concentrations at the downgradient property boundary within a reasonable timeframe when PFAS travel time is relatively slow. Among the CAC alternatives evaluated here, a downgradient CAC permeable reactive barrier has the best performance with respect to protecting downgradient receptors. [ABSTRACT FROM AUTHOR]