Carbon superstructures with graphitized lamellar microstructures were fabricated through a modified hydrothermal method. The dual oxidation process combining acrylic acid functionalization and air thermal treatment introduced plentiful carboxyl groups on the surface of the carbon superstructures. Adsorption capacity of U(VI) on the as prepared carbon superparticles reached 197.7 mg g(-1), which was 9-fold higher than that of raw glucose-derived hydrothermal carbon microspheres. The thermo-dynamic and kinetic studies demonstrated that the uptake of uranyl ions was a spontaneous and endothermic chemisorption dominated process with the abundant carboxyl groups acting as main binding sites. Impressively, the carbon superstructure adsorbents showed excellent recycling performance. To sum up, this paper proposed a novel high-performance U(VI) adsorbent from hydrothermal carbon, which exhibited potential in real application due to their outstanding reusability and scale-up capability.