Biphenyl, a frequently encountered and resilient compound in wastewater, proves resistant to conventional treatment methods because of its enduring nature. It forms the structural basis for persistent organic pollutants such as PCBs. In this study, we explored the adsorption of biphenyl in an organo-aqueous medium using both natural (Bent) and organomodified (CTAB-Bent) bentonite clay. Our objective was to highlight its potential for biphenyl wastewater treatment. We analyzed the physicochemical and textural properties of these clays through FTIR, XRF, XRD, SEM, BET method, and Zeta potential measurements. Impressively, these materials exhibited remarkable biphenyl adsorption capacity under acidic conditions, with Bent achieving 60% removal and CTAB-Bent an impressive 91%. We investigated the adsorption kinetics using first-order and pseudo-second-order models and assessed isotherm data with the Langmuir, Freundlich, and Langmuir-Freundlich (sips) equations. The Langmuir model, at pH 3, proved optimal, with high accuracy (R²) and minimal error (RMSE) values (0.997 and 1.20, respectively). Clay nature significantly influenced pollutant uptake efficiency, confirming the efficacy of the selected bio-based clay. We propose a protocol adaptable for industrial-scale applications.