A novel negatively charged thorium-iron oxo cluster， ［Th2Fe10O4（C6H5PO3）12（CH3O）8Cl4］6-（Th2Fe10） was synthesized via the solvothermal method. Multiple techniques were employed to investigate its structure， chemical compositions， magnetic properties and catalytic performance. Single-crystal X-ray diffraction data revealed that the structure of Th2Fe10 represents a novel dodecanuclear Th-Fe oxo cluster， which is formed due to the synergistic hydrolysis， alcoholysis and condensation reactions of Th（Ⅳ） and Fe（Ⅲ） ions， along with the passivation by phenylphosphonate groups. Th2Fe10 is not only the second reported Th-Fe oxo cluster， but also one of the few actinide-transition metal oxo clusters. The crystals of Th2Fe10 exhibit remarkable visible light absorption properties and strong antiferromagnetic exchange interactions between Fe（Ⅲ） ions. Moreover， Th2Fe10 possesses excellent performance in catalyzing the benzylamine coupling reaction， achieving up to 94% conversion and 96% selectivity， while maintaining good catalytic performance after multiple cycles. Scavenging experiments of reactive species demonstrated that electrons， holes， 1O2 and ·OH play significant roles in the catalytic process， which was further verified through electrochemical measurements and electron paramagnetic resonance（EPR） spectroscopy. The catalytic reaction mechanism was postulated based on these experimental results.
