“…[ 11,13–15 ] The operation of state‐of‐the‐art supercapacitor electrode materials consist of multiple electrochemical steps including the adsorptions of ions, the ions diffusion to active surface, redox reaction, and electrons charge transfer. [ 8,16–20 ] Layered double hydroxide (LDH) consist of metallic cations with multivalent states, interlayer anions, and water molecules for charge balance that stabilized as unique layered structures, [ 21–24 ] which have been extensity explored as the potential candidates for supercapacitors applications including NiCo, [ 14,25–28 ] NiMn, [ 29,30 ] CoMn, CoFe, and other doped systems. [ 31 ] In particular, Ni‐based LDHs have a fabulous theoretical specific capacitance of more than 3000 F g −1 .…”