In the present study, we propose a novel electrode material ofβ-nickel hydroxide covering nickel/aluminum lay-ered double hydroxides via a facile complexation-precipitation method. The as-obtained materials with 3-dimensional nanostructures are further utilized as highly capable electrode material in nickel-metal hydride bat-teries. The electrochemical test results demonstrated theβ-nickel hydroxide covering nickel/aluminum-layered double hydroxides with 28％ofβ-nickel hydroxide provided a superior specific capacity value of 452 mA·h·g?1 in a current density of 5 A·g?1 using 6 M KOH as electrolyte as compared with other materials. In addition, the optimized sample displays an outstanding cyclic stability along with a huge specific capacity value of 320 mAh·g?1, and very small decay rate of 3.3％at 50 A·g?1 after 3000 cycles of charge/discharge test. These in-dicate that the newly designed material with nanostructures not only provides an efficient contact interface be-tween electrolyte and active species and facilitates the transport of electrons and ions, but also protects the 3-dimensional nickel/aluminum layered double hydroxides, achieving a high specific capacity, fast redox reaction and excellent long-term cyclic stability. Therefore, theβ-nickel hydroxide covering nickel/aluminum layered double hydroxides with superior electrochemical performance is predictable to be a gifted electrode material in nickel-metal hydride batteries.