Phosphorus is a crucial element for living systems and plays significant roles in plant growth. The world’s supply of phosphorus today, however, relies on depleting feedstocks such as phosphate rocks, while the demand for phosphorus fertilizers escalates as the population continues to grow. It is thus urgent to develop sustainable sources and production methods for phosphorus. Here, we report on catalytic dephosphorylation for phosphorus recovery from organic and biological molecules. Ceria (CeO2) nanocrystals were synthesized with shape control and applied as artificial phosphatases to cleave the phosphate ester bond in para-nitrophenyl phosphate and release free phosphate anions in aqueous solutions. The dephosphorylation reaction was studied on the CeO2 nanocrystals at various temperatures to evaluate the dependences of rate constant, activation energy, and recyclability on the particle shape. The structure–property relationships established in these studies suggest that the oxygen vacancies on the surface of CeO2 are the active sites for dephosphorylation.