This study investigated a magnetically recycled modified polishing powder (CMIO@PP) as an adsorbent of phosphate; the CMIO@PP was synthesized by combining the modified La/Ce-containing waste polishing powder with CaO2-modified Fe3O4 (CMIO). Results indicate that the CMIO@PP nanocomposite presents a crystal structure comprising La (OH)3, Ce (OH)3, and Fe3O4, and that CMIO is uniformly dispersed in the modified polishing powder. The CMIO@PP (1:3) is a suitable choice considering its magnetism and adsorption capacity. The magnetic adsorbent exhibits a high adsorption capacity of 53.72 mg/g, a short equilibrium time of 60 min, and superior selectivity for phosphate. Moreover, the adsorbent strongly depends on the pH during the adsorption process and maintains a large adsorption capacity when the pH level is between 2 and 6. The adsorption of phosphate by the CMIO@PP (1:3) accords with the Langmuir isotherm model, and the adsorption process follows the pseudo-second order model. Meanwhile, adsorption–desorption experiments show that the adsorbent could be recycled a few times and that a high removal efficiency of phosphate from civil wastewater was achieved. Finally, mechanisms show that the adsorption of phosphate by the CMIO@PP (1:3) is mainly caused by electrostatic attraction and ligand exchange.