Capacitive deionization has been considered as a promising wastewater treatment technology because of its low-cost and highly efficient. Herein, we prepared hollow bowl-type carbon materials loaded with molybdenum sulfide (HBC-MoS2) composites and fabricated it as an innovative electrode material to remove Cu2+ in a multi -ion coexistence system. With the synergistic effect of electric double layer (EDL) and complexation between MoS2 and Cu2+, the HBC-MoS2-0.02 electrode achieved effective removal of copper ions from low concentration wastewater (25 mg/L) and high electrosorption capacity of 28.97 mg g-1 at 1.0 V. Even in the presence of competing ions (Na+/Zn2+/Cu2+), the HBC-MoS2-0.02 electrode still can effectively remove Cu2+ with a final adsorption capacity of 28 mg g-1, showing its superiority. The mechanism of Cu2+ removal by HBC-MoS2 is mainly due to the synergistic effect of EDL and complexation.