We report the optimized preparation by liquid phase deposition (LPD) of nickel–aluminum layered double hydroxide/carbon (Ni–Al LDH/C) composites as nickel-based cathode materials. We investigate the influence of the LDH content on the properties of the composites prepared with various total volumes of the reaction solution while the solution composition and the amount of carbon are maintained constant. Diffraction patterns show that the crystallinity of the composite increases with increasing the LDH content. Gravimetric studies indicate that there is no correlation between the amount of the deposit and the total volume of the reaction solution. Inductively coupled plasma-atomic emission spectroscopy (ICP-AES) reveals that the optimal Al3+/(Al3+ +Ni2+) is obtained for the sample with the highest LDH content. The optimized composition results in high performance cathode materials; a high discharge capacity (>390mAhgcomp −1) at the 1.0 C-rate, a good cycle life at 2.0 C-rate over 300 cycles and excellent electrochemical stability.