The synthesis of battery-type electrode materials with hollow nanostructures for high-performance hybrid supercapacitors (HSCs) remains challenging. In this study, hollow CuS@Ni-Co layered double hydroxide (CuS-LDH) composites with distinguished compositions and structures are successfully synthesized by co-precipitation and the subsequent etching/ion-exchange reaction. CuS-LDH-10 with uniformly dispersed CuS prepared with the addition of 10 mg of CuS shows a unique hollow polyhedral structure constituted by loose nanosphere units, and these nanospheres are composed of interlaced fine nanosheets. The composite prepared with 30 mg of CuS addition (CuS-LDH-30) is composed of a hollow cubic morphology with vertically aligned nanosheets on the CuS shell. The CuS-LDH-10 and CuS-LDH-30 electrodes exhibit high specific capacity (765.1 and 659.6 C g