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Capacitive deionization (CDI) technology holds great potential for rapid and efficient uranyl ion removal from wastewater. However, the related electrode materials still have much room for research. Herein, chitosan/phytic acid complexes were anchored on polypyrrole nanotubes (CS/PA-PPy) to fabricate the electrode for the electrosorption of uranyl ions (UO 2 2+). In this system, polypyrrole nanotubes provided specific channels for ion and electron diffusion, and chitosan/phytic acid complexes offered selective sites for UO 2 2+ binding. The results demonstrated that CS/PA-PPy via electrosorption showed faster kinetics and higher uranium uptake than those via physicochemical adsorption. The maximum adsorption capacity toward UO 2 2+ via electrosorption (1.2 V) could reach 799.3 mg g−1, which was higher than most of the reported CDI electrodes. Electrochemical measurements and experimental characterizations showed that the electrosorption of UO 2 2+ by CS/PA-PPy was a synergistic effect of capacitive process and physicochemical adsorption, in which the capacitive mechanism involved the formation of an electric double layer from hollow polypyrrole nanotubes, whereas the coordination of phosphate, amino and hydroxyl groups with UO 2 2+ was attributed to physicochemical adsorption. With the rational design of material, along with its excellent uranium removal performance, this work exhibited a novel and potential composite electrode for uranium capture via CDI from wastewater. Chitosan/phytic acid complexes were anchored on polypyrrole nanotubes to fabricate capacitive deionization electrode for the removal of uranyl ions from wastewater. [Display omitted] [ABSTRACT FROM AUTHOR]