A wet loading method was developed to produce nano-sized LiBH4 combined with nano-SiO2 templates. The multicomponent LiBH4/SiO2 material synthesized by the wet method has been found to dehydrogenate at much lower temperatures than the pure LiBH4, as well as LiBH4/SiO2 mixtures prepared by ball milling. For example, the onset of dehydrogenation was decreased to about 200 °C for a wet-treated LiBH4/SiO2 mixture with a mass ratio of 1:1, and the majority of the hydrogen could be released below 350 °C. The improved dehydrogenation of the wet-treated LiBH4/SiO2 mixtures can be attributed to the destabilization of SiO2, resulting in the formation of lithium metasilicate (Li2SiO3) upon heating, and the confinement of LiBH4 to form nanoscale particles.