• • ECUT-COF-152 achieves 100% U(VI) removal and a maximum reduction capacity of 1950 mg g−1 under visible light, outperforming many reported photocatalysts and enabling efficient uranium recovery from wastewater.
• • The D-A architecture with TP as donor and 1,4-DQ/1,5-DQ as acceptors extends electron transfer distance, reducing electron-hole recombination and boosting photocatalytic efficiency.
• • The design eliminates the need for additional functional groups, simplifying synthesis while maintaining high crystallinity and porosity, which is critical for scalable production.
• • The work provides a clear structure-property relationship: adjusting the connection mode of building units directly modulates electron transport, offering a general strategy for designing high-performance COF photocatalysts.