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One of the key factors to improve electrochemical properties is to find exceptional electrode materials. In this work, the nickel-cobalt layered double hydroxide (CNT@CoS/NiCo-LDH) with the structure of a hollow nanocage was prepared by etching CNT@CoS with zeolitic imidazolate framework-67 (ZIF-67) as a template. The results show that the addition of nickel has a great influence on the structure, morphology and chemical properties of materials. The prepared material CNT@CoS/NiCo-LDH-100 (C@CS/NCL-100) inherited the rhombic dodecahedral shape of ZIF-67 well and the CNTs were evenly interspersed among the rhombic dodecahedrons. The presence of CNTs improved the conductivity and surface area of the samples. The C@CS/NCL-100 demonstrates a high specific capacitance of 2794.6 F·g−1 at 1 A·g−1. Furthermore, as an assemble device, the device of C@CS/NCL-100 as a positive electrode exhibits a relatively high-energy density of 35.64 Wh·kg−1 at a power density of 750 W·kg−1 Further, even at the high-power density of 3750 W·kg−1, the energy density can still retain 26.38 Wh·kg−1. Hence, the superior performance of C@CS/NCL-100 can be ascribed to the synergy among CNTs, CoS and NiCo LDH, as well as the excellent three-dimensional structure obtained by used ZIF-67 as a template. [ABSTRACT FROM AUTHOR]