A simple synthetic method without organic template is proposed for the synthesis of Ni-silicate. The resulting Ni-phyllosilicates are reconstructed by hydrothermal treatment to a porous structure with a high surface area (552 m(2)g(-1)). Notably, the residual filtrate has a Ni(2+)ion content of less than 0.1 ppm, and therefore satisfies the effluent standard in Taiwan (<1.0 ppm). As a result, it can be disposed of directly without the need for additional treatment. The effects of the pH value and hydrothermal treatment time on the structure, morphology, and surface area of the Ni-silicate composites have been investigated. When applied to hydrogen production, the mesoporous Ni-silicate shows a high catalytic capability (>99%) toward ammonia decomposition at a temperature of 400 degrees C. Overall, the proposed synthetic method is facile and easily extendable to the production of other metal-silicate materials for hydrogen generation.