In this study, Ce⁴⁺-doped Ni–Al mixed oxides (NACO) were synthesized and comprehensively characterized for their potential application in fluoride adsorption. NACOs were examined using Transmission Electron Microscopy (TEM) and Scanning Electron Microscopy (SEM), revealing a sheet-like morphology with a nodular appearance. X-ray diffraction (XRD) analysis confirmed the formation of mixed oxides of cubic crystal structure, with characteristic planes (111), (200), and (220) at 2θ values of 37.63°, 43.61°, and 63.64°, respectively. Further investigations using X-ray Photoelectron Spectroscopy (XPS) identified the presence of elements such as Ni, Al, Ce, and O with oxidation states +2, +3, +4, and −2, respectively. The Brunauer–Emmett–Teller (BET) analysis indicated that NACO followed a type IV physisorption isotherm, suggesting favorable surface adsorption characteristics. The adsorption kinetics was studied, and the experimental data exhibited a good suit to both pseudo-first order and pseudo-second order, as indicated by high R² values. Moreover, the Freundlich isotherm model demonstrated a good fit to the experimental data. The result also revealed that NACO has a maximum capacity for adsorption (q_max) of 132 mg g⁻¹. Thermodynamic studies showed that fluoride adsorption onto NACO was feasible and spontaneous. Additionally, NACO exhibited excellent regeneration capabilities, as evidenced by a remarkable 75.71% removal efficiency at the sixth regeneration stage, indicating sustained adsorption capacity even after multiple regeneration cycles. Overall, NACOs displayed promising characteristics for fluoride adsorption, making them potential candidates for efficient and sustainable water treatment technologies.