Seeking highly efficient and low-cost sorbents to removal uranium contaminants is of great concern in demand. In present work, a graphene oxide sponge (GOS) was successfully assembled by a facile Ethylenediaminetetraacetic acid (EDTA)assisted hydrothermal method from graphene oxide (GO) sheets. The prepared GOS was characterized, and the influencing factors on uranium sorption were optimized. Results indicate that the GOS shows a spongy porous structure and significantly enhances the U(VI) removal compared with the pristine GO. Langmuir model well describes the equilibrium sorption data. Under experimental conditions, the maximal uranium sorption calculated from Langmuir model was found to be 212.77 mg . L-1. Sorption kinetics data are matched with pseudo-second-order model. Reusability experiments indicate that the prepared GOS can be regenerated using dilute acid treatment and be used repeatedly. The simple and low-cost preparation of GOS predicts the potential applications of spongy GO as an effective sorbent for U(VI) capture and also expands the possibility of using graphene-based sorbent in the disposal of liquid radioactive waste. Copyright c 2016 John Wiley & Sons, Ltd.