Three-dimensional cubic ordered mesoporous carbon with chitosan (Ia3d-CS), which was synthesized via exothermic reaction between liquid potassium and carbon monoxide gas, was coated on the active carbon (AC) electrode as a capacitive deionization (CDI) disinfection electrode. The results showed that Ia3d-CS-2 as CDI electrode exhibited the quick ion diffusion and strong charge transfer performance, due to the three-dimensional pore structure and specific surface area. The electrode of Ia3d-CS-2 displayed a specific capacity of 191.22 F/g at a scan rate of 100 mV·s^-1 in 0.5 M NaCl aqueous solution. In a CDI recycling system, Ia3d-CS-x electrode showed good cyclic stability, and the electrosorption capacity of Ia3d-CS-2 electrode can achieve 1.31 mg/g at 1.2 V in 100 mg/l NaCl aqueous solutions. Subsequently, Ia3d-CS-2 electrode had an excellent disinfection efficiency of killing about 99.99% Escherichia coli within 30 min during the CDI process at applied 1.2 V. Considering those excellent properties of the fabricated Ia3d-CS-x electrode, which should be a better candidate for high-performance deionization application.