Layered double oxides (LDOs) samples derive from layered double hydroxides (LDHs) by thermal treatment at different temperatures are prepared in this paper. The as-prepared LDOs samples are characterized by X-ray diffraction (XRD), thermogravimetry-differential thermal analysis (TG-DTA) and scanning electron microscope (SEM) technique. The results show that the LDHs are decomposed to ZnO with amorphous aluminium species dispersed in the lattice. After calcinations, LDOs inherit the lamellar structure of LDHs. LDOs with thermal treatment at different temperature are tested as the anode active materials for Zn/Ni secondary battery. Cyclic voltammetries (CV) and Tafel curves measurements reveal that the calcined products have better electrochemical performances, lower polarization and better reversibility. Galvanostatic charge/discharge shows that the calcined products have excellent cycle stability and higher specific discharge capacity. More interesting, the sample calcined at 500°C exhibits the best electrochemical performances among all samples. These findings promote new opportunities for anode materials as Zn/Ni batteries and other energy-storage devices.