ZnO/Polypyrrole (PPy) composites are synthesized by ultrasound assisted chemical polymerization of PPy in the presence of ZnO particles. With different initial content of pyrrole, granular and layered ZnO/PPy composite are formed. The fourier transform infrared spectra (FT-IR), X-ray diffraction (XRD), scanning electron microscopy (SEM) and transmission electron microscopy (TEM) are adopted to characterize the as-prepared samples. ZnO/PPy composites are used as anode material for Zn/Ni batteries. Galvanostatic charge/discharge experiments, cyclic voltammograms (CV) and electrochemical impedance spectroscopy (EIS) are conducted to evaluate the cycle performance of electrodes. ZnO/PPy composites show superior capacity stability, more stable charge plateau and higher discharge plateau compared to conventional ZnO electrode. Furthermore, rate performance is also improved by ZnO/PPy composites.