Zn–Al–In layered double hydroxides (LDHs) are synthesized by hydrothermal method and investigated as negative electrode materials for Ni–Zn batteries. The Fourier transform infrared spectra (FT-IR), X-ray diffraction (XRD), scanning electron microscopy (SEM) and transmission electron microscopy (TEM) images show the as-prepared samples are well-crystallized and hexagon structure. The electrochemical performances of Zn–Al-LDHs and Zn–Al–In-LDHs with different Zn/Al/In molar ration are investigated by the cyclic voltammograms (CV), Tafel polarization and galvanostatic charge–discharge measurements. Zn–Al-LDHs shows good stability in the first 300-cycles. However, during the subsequent cycles, the discharge capacity decreases with increasing of the cycles. Compared with Zn–Al-LDHs, Zn–Al–In-LDHs with different Zn/Al/In molar rations, especially the sample of Zn/Al/In = 3:0.75:0.25 (molar ration) have higher discharge capacity and more stable cycling performances. This battery can undergo at least 800 charge–discharge cycles at constant current of 1C without dendrite and short circuits. The discharge capacity of Zn–Al–In-LDHs after the 800th cycle remains about 380 mAh g−1. Zn–Al–In-LDHs possess a high rate capability to meet the needs of high-storage applications.