Abstract Efficient uranium extraction is crucial for sustainable environmental remediation. Zirconium‐based porphyrin metal‐organic frameworks (MOFs) emerge as promising photocatalysts for this purpose. Herein, a series of magnetic core‐shell photocatalysts (MNPs@PN‐PCN‐222, MNPs@PN‐PCN‐223, and MNPs@PN‐MOF‐525) is prepared via a one‐pot solvothermal approach, functionalized with phosphate groups (PN) for uranium affinity. Comprehensive characterization confirms successful PN grafting onto MOF surfaces and reveals a pronounced redshift in optical absorption to ≈700 nm due to MNP incorporation, significantly enhancing visible‐light harvesting. Under visible irradiation, MNPs@PN‐PCN‐222 achieves a record uranium adsorption capacity of 1.2 g g −1 (62% extraction efficiency), representing a 9.3 times enhancement over dark conditions. The photocatalyst maintains >80% efficiency over four reuse cycles, demonstrating exceptional stability and magnetic recoverability. This work establishes a generalizable platform for designing high‐performance, recyclable zirconium‐porphyrin photocatalysts for nuclear wastewater treatment.