Excessive nitrogen (N) and phosphorus (P) result in serious eutrophication of water. In this study, magnesium modified acid bentonite was prepared by the impregnation method, and nitrogen and phosphorus were simultaneously removed by the magnesium ammonium phosphate method (MAP), which solved the problem of the poor adsorption capacity of bentonite. The morphology and structure of MgO-SBt were characterized by XRD, FT-IR, SEM, EDS, XPS, BET, etc. The results show that the acidified bentonite can increase the distance between bentonite layers, the layer spacing is expanded to 1.560 nm, and the specific surface area is expanded to 95.433 m2/g. After Mg modification, the characteristic peaks of MgO appear at 2θ of 42.95°, 62.31°, and 78.72°, indicating that MgO has been successfully loaded and that MgO bonded to the surface and interior pores of the acidified bentonite, boosting adsorption performance. When the dosage of MgO-SBt is 0.25 g/L, pH = 9, and N/P ratio is 5:1, the maximum adsorption capacity of MgO-SBt for N and P can reach 193.448 mg/g and 322.581 mg/g. In addition, the mechanism of the simultaneous adsorption of nitrogen and phosphorus by MgO-SBt was deeply characterized by the kinetic model, isothermal adsorption model, and thermodynamic model. The results showed that the simultaneous adsorption of nitrogen and phosphorus by MgO-SBt was chemisorption and a spontaneous exothermic process.