This study investigates dual-functional ball-milled Clay-Fe-Ti composites for efficient adsorption and photocatalytic regeneration of Ni(II), Pd(II), and Pt(II) ions. The nanocomposite achieved 79.5% removal efficiency for mixed metal ions, with a maximum adsorption capacity of 65.4 mg/g. Optimal conditions were determined via ANN-GA optimization: pH 3.5, 46.8°C, 5.9 g/L Clay-Fe-Ti, 37 W lamp power, and 3.7 g/L calixarenes on XAD. Adsorption followed the Freundlich isotherm (heterogeneous interactions) and Fractal-like-pseudo-first-order kinetics. Density functional theory (DFT) confirmed the material’s stability and adsorption mechanisms. Combining experimental design (RSM) with computational modeling (ANN-GA), the composite demonstrates regenerable photocatalytic activity after metal uptake, enabling repeated cycles. These results highlight Clay-Fe-Ti as a sustainable, cost-effective solution for heavy metal remediation, bridging adsorption and catalytic degradation in wastewater treatment.