A zirconium-based metal-organic framework (DUT-69) was fabricated via a hydrothermal synthesis for U(VI) removal in aqueous solutions. Experimental results showed that the maximum adsorption capacity for U(VI) was 362.32 mg center dot g(-1) at 303 K, pH = 6 and initial U(VI) concentration of 80 mg L-1. The adsorption process fit well with the pseudo-second-order kinetic and Langmuir models. Various characterizations indicated that complexation interactions was the central adsorption mechanism and electrostatic was the secondary. The carboxyl, Zr-O, and C-S bonds in the framework participated i...