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Combining adsorption with other technologies holds great potential in fast and deep arsenic ion removal. Herein, chitosan‑zirconium composite adsorptive membranes (CS-Zr CM) were successfully prepared using simple casting and sodium hydroxide coagulation strategies, which was demonstrated the use in arsenic ion-capture electrodialysis based on their good adsorption performance. In the batch adsorption tests, the maximum adsorption capacities of CS-Zr CM for As(III) and As(V) were 134.2 mg/g and 119.5 mg/g, respectively. CS-Zr CM also exhibited satisfying adsorption selectivity and good reusability toward As(III) and As(V). However, the adsorption kinetics showed that they needed 48 h to reach the adsorption equilibrium and the adsorption ability toward trace arsenic ion was ineffective. Furthermore, CS-Zr CM was applied as the adsorptive membrane in the electrodialysis process. Under the influence of electric field, the As(III) and As(V) removal equilibrium time was shortened to 12 h and the concentrations of As(III) and As(V) ions could be efficiently reduced to below the WHO limit in drinking water (10 μg/L), which far surpassed the physicochemical adsorption method. Such good arsenic ion removal ability of CS-Zr CM together with the ease scalable fabrication, low cost, and biodegradable properties shows its huge prospects in arsenic-containing wastewater treatment. Biodegradable chitosan‑zirconium composite adsorptive membrane was used in the arsenic ion-capture electrodialysis configuration which exhibited fast and deep arsenic ion (As(III) and As(V)) removal. [Display omitted] [ABSTRACT FROM AUTHOR]