It has been well accepted that the performance of supercapacitor material highly depends on its morphology, thus the control on morphology is significant for acquiring advanced materials. Herein, a facile method for controllable synthesis of nickel-cobalt layered double hydroxide (Ni-Co LDH) with a unique hollow structure is presented. In which zeolitic imidazolate framework-67 (ZIF-67) nanocrystals are used as templates and etched in a nitrate solution. The morphology of Ni-Co LDH shows an interesting variation with a different dosage of Ni(NO3)2. The Ni-Co LDH with integrated hollow structure exhibits superior electrochemical property among the obtained materials. The electrochemical tests revealed that the electrode display a specific capacity of 790Cg−1 at 2Ag−1 and a favourable rate capability. The integrated polyhedral hollow structure and the interlaced nanosheets make the Ni-Co LDH a highly promising material for hybrid supercapacitors.