Consumption of food and water contaminated with PFOA (perfluorooctanoic acid) and PFOS (perfluorooctanesulfonic acid) presents a potential human health risk. There is limited data on high affinity sorbents that can be used to decrease the bioavailability of per- and polyfluoroalkyl substances from soil and translocation to plants and garden produce. To address this need, montmorillonite clay was amended with the nutrients carnitine and choline to increase the hydrophobicity of the sorbent and the interlayer spacing. In this study, the binding of PFOA and PFOS to parent and amended clays was characterized. Isothermal analyses were conducted at pH 7 and ambient temperature (to simulate environmentally relevant conditions). The data for all tested sorbents fit the Langmuir model indicating saturable binding sites with high capacities and affinities under neutral conditions. Amended montmorillonite clays had increased capacities for PFOA and PFOS (0.51 – 0.71 mol kg-1) compared to the parent clay (0.37 – 0.49 mol kg-1). Molecular dynamics (MD) simulations suggested that hydrophobic and electrostatic interactions at the terminal fluorinated carbon chains of both PFAS compounds were major modes of surface interaction. The safety and efficacy of the clays were confirmed in a living organism (Lemna minor), where clays (at 0.1% inclusion) allowed for increased growth compared to PFOA and PFOS controls (p ≤ 0.01). Importantly, soil studies showed that 2% sorbent inclusion could significantly reduce PFOA and PFOS bioavailability from soil (up to 74%). Studies in plants demonstrated that inclusion of 2% sorbent significantly reduced PFOA and PFOS residues in cucumber plants (p ≤ 0.05). These results suggest that nutrient-amended clays could be included in soil to decrease PFOA and PFOS bioavailability and translocation to plants.