Supported NiO nanoparticles (NPs) were prepared by impregnation of mesoporous silica SBA-15 with a molecular, metalorganic [Ni₄O₄] cubane cluster as precursor. By using this ligand-stabilized Ni cluster, deposition of four Ni ions in close proximity on the silica support was achieved; this resulted in the formation of small and highly dispersed NiO NPs after heat treatment. These clusters were shown to have a significant influence on the formation of NiO NPs compared to a conventional Ni(OAc)₂ precursor. After a further reduction step, the materials were used as catalysts for the dry reforming of methane, which showed that preorganization of the Ni atoms on the support surface had a beneficial effect on the methane conversion rate.