In this research work, new composite materials based on magnesium phosphate cement (MPC) were developed to evaluate the retention of fluorine from wastewater. This material was prepared with dead burned magnesia oxide (MgO), ammonium dihydrogen phosphate (NH4H2PO4), and some retarding agents. We chose to synthesize with hydrogen peroxide instead of water; alumina and zeolite were also added to the cement. The obtained optimal conditions were studied and analyzed by X-ray diffraction (XRD) and scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), BET, and thermogravimetric analysis (TGA). The adsorbents showed a strong ability to remove fluoride from contaminated water, and the best defluoridation capacity was evaluated as 2.21 mg/g for the H2O2 cement. Equilibrium modeling was performed, and the experimental data were presented according to the isotherms of Langmuir, Freundlich, Temkin, and Dubinin–Radushkevich.