Highly efficient extraction of radioactive uranium from aqueous solution remains a serious task in the nuclear energy field. To address this, we here create an effective uranium ion trap by using a novel and facile strategy that introduces bioinspired moiety phytic acid (PA) into highly robust PCN-222. The resultant metal–organic framework (MOF)-based uranium ion trap (PCN-222-PA) with a high density of accessible phosphate groups exhibits a remarkable U(VI) uptake capacity (401.6 mg·g–1), surpassing most of the reported phosphorus-modified MOFs and various other MOF adsorbents. Kinetics study reveals that PCN-222-PA can reduce the uranium concentration from 10 mg L–1 to 21 μg L–1, below the acceptable limit defined by the US Environmental Protection Agency. In addition, PCN-222-PA also shows good selectivity and high stability as well as excellent recyclability toward uranium capture. Our work demonstrates a new strategy to design functional MOFs with abundant phosphate groups and provides a new perspective for extracting uranium from aqueous solution.