Electrochemical supercapacitors (SCs) are high-efficiency electrochemical energy storage devices that can deliver energy at a very fast rate. Metal− organic framework (MOF)-derived layered double hydroxides (LDHs) are promising materials with great potential for commercial SC applications. In this study, a two-step synthetic strategy was developed to produce porous nanostructured ZnCoNi-LDH nanosheets (NSs) from bimetallic MOFs through a chemical reduction method. All the as-synthesized materials were characterized for their crystal structure, phase, morphology, and surface construction. The optimized ZnCo 2 Ni-LDH composition exhibited the best charge storage ability and specific capacitance among the different assynthesized compositions. The specific capacitance of the fabricated device ZnCo 2 Ni-LDH||cellulose paper-KOH||ZnCo 2 Ni-LDH was found to be 348.2 F g −1 at 1.0 A g −1 , with a maximum energy density of 54.4 W h kg −1 and a power density of 4439.0 W kg −1 . After 10,000 continuous charge−discharge cycles, the device retained 86% of its capacitance. It also delivered a high-capacitance-specific Coulombic efficiency (57−60%). A mechanistic study corroborated the experimental results that the high pore volume, possible insertion of a greater number of electrolyte ions, multioxidation states of Ni and Co ions, and their synergistic effect with Zn 2+ all contributed to the diffusion-controlled charge storage behavior. The charge storage characteristics of the device were found to be a combination of redox and electrostatic effects, forming a facile hybrid SC.