Silver-coated layered double hydroxide (Ag-coated LDH) nanosheets are successfully prepared by a facile silver mirror reaction and their electrochemical performance has been evaluated as anode materials for Ni–Zn secondary batteries. The microstructure and morphology of as-prepared Ag-coated Zn/Al-LDH are investigated by scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray diffraction (XRD). As anode material for Ni–Zn secondary batteries, Ag-coated Zn/Al-LDH exhibits high specific capacity (400 mAh g−1), good charge–discharge properties and excellent cycling performance, which is attributed to the effect of the electron conductivity improvement by the Ag coating on the surface of Zn/Al-LDH nanosheet. This newly designed Ag-coated Zn/Al-LDH may offer a promising anode candidate for high-performance Ni–Zn secondary batteries.