In this work, Zn–Al layered double oxides (Zn–Al-LDO) were prepared via a facile hydrothermal method, followed by calcination treatment in an air atmosphere, and evaluated as anode materials of Zn/Ni batteries. The morphology and structure of as-prepared Zn–Al-LDO and its precursor Zn–Al layered double hydroxide (Zn–Al LDH) were investigated through Fourier transform infrared spectra (FT-IR), X-ray diffraction (XRD), scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Compared to the Zn–Al-LDH precursor, Zn–Al-LDO possesses higher discharge capacity, better reversibility and longer cycle life. The discharge capacity of Zn–Al-LDO remains about 460 mA h g⁻¹ after 1000 cycles. In particular, good rate performance can be observed for a Zn–Al-LDO electrode. The superior properties could be ascribed to improved charge conductivity and the absence of carbonate anions, which make migration of hydroxyl anions smooth to meet the requirements of the electrochemical reaction of the electrode.