Ni_1/3Co_2/3(CO₃)_1/2(OH)·0.11H₂O (NCC) was in situ constructed on the surface of CNTs, which realized the nanoscale recombination of NCC and CNTs. The as-obtained CNTs@NCC composite showed excellent electrochemical performance in both aqueous and all-solid-state electrolyte systems owing to the improvement in the utilization of active materials. This work provides a general duty strategy for improving the combined electrochemical performance of electrode materials for energy storage.