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• Floriform WO 3 /C electrode were developed for electrosorption of U(VI) from water. • The charge/discharge process of WO 3 /C primarily belongs to capacitive controlled behavior. • WO 3 /C electrodes achieve a maximum U(VI) electrosorption capacity of 449.9 mg g−1 at 1.2 V. • Electrosorption of U(VI) is credited to synergistic effect of EDLs and pseudocapacitance from WO 3 /C. Decontamination and recovery of uranium(VI) [U(VI)] from radioactive wastewater is vital to sustainable nuclear power production and reclamation of radioactive waste. As a promising technology of water treatment, capacitive deionization for adsorption of U(VI) started to attract attention. Herein, for the first time, a floriform WO 3 /C composite was developed as a pseudocapacitive electrode material for electrosorption of U(VI) from water. The as-prepared WO 3 /C composite was constructed from dozens of 2D nanosheets with a thin amorphous carbon layer, resulting in uniform flower-like particles with hierarchical nanostructure and superior open pore network. The charge/discharge process of WO 3 /C was demonstrated as prominent capacitive controlled behavior by quantization of capacitance contributions. As a result, the WO 3 /C electrodes achieved a maximum U(VI) electrosorption capacity of 449.9 mg g−1 at 1.2 V and good cycling stability after consecutive adsorption-desorption, which is superior to the conventional physical adsorption processes. The superior CDI performance of the WO 3 /C electrode is credited to the synergistic effect of EDLs and pseudocapacitance based on the combination of WO 3 and carbon layer with hierarchical nanostructure. Overall, the facile preparation strategy, the superior electrosorption performances, and the high cycling stability, endow the floriform WO 3 /C electrodes to be a promising electrode material for electrosorption of U(VI) from wastewater. [ABSTRACT FROM AUTHOR]