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Our photocatalyst possesses homo/heterojunction structure, which consists of hexagonal CdS, cubic CdS and Prussian blue. This design of homo/heterojunction structure not only achieves ideal energy band structure, which makes for stable and rapid separation of photogenerated electrons-holes, but also improves stability of photocatalyst in various extreme circumstances. Therefore, the photocatalytic activity is significantly enhanced. [Display omitted] • The homo/heterojunctions structures were designed via one-pot kinetic regulation. • The rational energy band distribution enhances photocatalytic activity. • The strong chelation between cyanogroups and Cd2+ improve the stability. • The photocatalysts possess excellent reusability. Photoreduction of soluble U(VI) to insoluble U(IV) by CdS-based catalysts shows great potential in remediating radioactive wastewater in terms of environmental friendliness and desirable bandgap as well as the availability of CdS, but is still limited by undesirable efficiency and stability from photogenerated carrier recombination and photocorrosion. Herein, we have elegantly designed tailor-made CdS@Prussian blue with homo/heterojunctions via one-pot kinetic regulation. The key to such a structure is to leverage the outstanding binding affinity between cyanogroups of Prussian blue and Cd2+ to create diversity of local precursor concentration differences. With such unique structure and rational energy band distribution, our photocatalysts demonstrate an unprecedented U(VI) removal efficiency as high as 2.5 times that of the pristine CdS. More importantly, the strong chelation between cyanogroups and Cd2+ endows our catalysts with extremely excellent stability compared with other state-of-the-art composite photocatalysts. This work provides a facile and universal inspiration for homo/heterojunction engineering of high-performance photocatalysts for photoreduction of uranium. [ABSTRACT FROM AUTHOR]