In this work, nanoporous cerium (Ce)-doped Febased MOFs were successfully synthesized by a convenient solventthermal method, which was designed to efficiently remove phosphate. Adsorption experiments showed that doping Ce into MIL-53(Fe)-NH 2 greatly improved its adsorption performance for phosphate. The maximum phosphate adsorption capacities of MIL-53(Fe)-NH 2 , 0.5Ce-MIL-53(Fe)-NH 2 , and Ce-BDC-NH 2 were 213.0 mg g −1 , 301.5 mg g −1 , and 246.0 mg g −1 , respectively. Moreover, they all had fast kinetics, and it took 80, 80, and 30 min for MIL-53(Fe)-NH 2 , 0.5Ce-MIL-53(Fe)-NH 2 , and Ce-BDC-NH 2 to reach equilibrium, respectively. Mechanism studies show that doping Ce with a larger ionic radius in MIL-53(Fe)-NH 2 increases the number of unsaturated coordination centers and defects in MOF crystals, resulting in more active sites for phosphate adsorption. Phosphate adsorption by 0.5Ce-MIL-53(Fe)-NH 2 includes ligand exchange and electrostatic attraction. In this process, Ce−O−P and Fe−O−P complexes are formed between phosphate and metal central ions, and surface hydroxyl groups play an important role. In addition, nanoporous bimetallic 0.5Ce-MIL-53(Fe)-NH 2 proved to be stable over a wide pH range and could be recycled at least 4 times. A low solid-to-liquid ratio of 0.5Ce-MIL-53(Fe)-NH 2 could remove phosphate from real wastewater, which exhibited excellent removal performance, excellent environmental adaptability, and high selectivity. All of the results indicate that bimetallic nanoporous 0.5Ce-MIL-53(Fe)-NH 2 is an outstanding phosphate adsorbent that could be potentially used to treat wastewater with significant application value in environmental remediation.