We report the durability of the optimized nickel–aluminum layered double hydroxide/carbon (Ni–Al LDH/C) composite prepared by liquid phase deposition (LPD) as cathode active materials in nickel metal hydride (Ni–MH) secondary battery. The positive electrode was used for charge–discharge measurements under two different current: 5 mA for 300 cycles in half-cell conditions, and 5.8 mA for 569 cycles in battery regime, respectively. The optimized Ni–Al LDH/C composite exhibits a good lifespan and stability with the capacity retention above 380 mA h gcomp −1 over 869 cycles. Cyclic voltammetry shows that the α-Ni(OH)2/γ-NiOOH redox reaction is maintained even after 869 cycles, and the higher current regime is beneficial in terms of materials utilization. X-ray diffraction (XRD) patterns of the cathode after charge and discharge confirms that the α-Ni(OH)2/γ-NiOOH redox reaction occurs without any intermediate phase.