Hydrocalumites additives are synthesized and proposed as an anodic additive for Zinc/Nickel alkaline secondary batteries. The as-prepared additives are characterized by Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD) and scanning electron microscopy (SEM). And the results illustrate that hydrocalumites additives are successfully prepared and have the typical structure of layered double hydroxides (LDHs). The effects of hydrocalumites additives on electrochemical performances of ZnO have been investigated by cyclic voltammetry (CV), tafel polarization tests, electrochemical impedance spectroscopy (EIS) and galvanostatic charge and discharge. Compared to the electrode with pure ZnO, the electrodes containing hydrocalumites additives show better reversibility, reveal better anti-corrosion property and exhibit more stable cycle performance. Especially when the electrode added with 12% (wt.) hydrocalumites, it exhibits the best cycle performance than the other electrodes. And its discharge capacity is about 450mAhg−1 all the time, and hardly declines over all the 400 cycles. Based on these observations, the prepared hydrocalumites may be a promising and efficient additive for the ZnO electrode.