A simple urea hydrothermal method was used to synthesize hollow spherical zinc-aluminum hydrotalcites (ZAL-H) with the particle size of about 6.7-9.8 mu m. The studies on different synthetic conditions have shown that the amount of urea and the type of solution system play important roles on the morphology and particle size of ZAL-H. X-ray diffraction (XRD) patterns indicate that thematerial has characteristic diffraction peaks of zinc-aluminum hydrotalcite. The specific surface area and pore size analysis (BET) indicate that the material has a uniform and narrow distribution of pore diameter of 3.682 nm and a specific surface area of 49.09 m(2) g(-1). As negative electrode material for zinc-nickel battery, the ZAL-H electrode exhibits a significantly enhanced discharge specific capacity compared to most previously reported electrodes based on zinc-aluminum hydroxides. The average discharge special capacity is 393.342 mAh g(-1) during the whole charge/discharge process (1050 cycles), the discharge efficiency is up to 97.34%, and the capacity retention rate is as high as 95.37%. Therefore, the ZAL-H is an excellent electrode active material and can be potentially applied to the energy storage/conversion devices. (C) 2019 The Electrochemical Society.