The nano-MOF+ technique was employed by assembling nanoporous metal-organic framework (MOF) UiO-66 with nanoscale zero-valent iron (ZVI) particles to remove uranyl ions from aqueous solution under anoxic condition for the first time. The synthesized composite of Fe0@UiO-66-COOH exhibits a synergic effect between uranyl sorption by MOF host of UiO-66-COOH and chemical reduction by ZVI, reaching much elevated removal capacity and rate in comparison to those of the pristine UiO-66-COOH. The combined complexation and reduction mechani**s are further elucidated by the synchrotron radiation X-ray absorption near-edge structure ****ysis. This work highlights the bright future of the nano-MOF+ technique in the application of uranium removal, especially for the remediation of the uranium-contaminated subsurface environment.