This study investigates the replacement of a costly commercial silicate source with locally abundant desert sand in the United Arab Emirates (UAE), for synthesizing mesoporous silica. Hydrothermal synthesis methods were employed to develop various mesoporous materials having different pore geometries, namely MCM41-S, SBA15-S and MCF-S, using desert sand as a silica source. These materials were then impregnated with 15 wt% NiO (∼13 wt% Ni) by sono-wet impregnation technique. All Ni-based silica supported catalyst demonstrated enhanced stability at 550 °C during the reaction. It was observed that the synthesized MCF-S proves to be a highly efficient catalyst support, as Ni/MCF-S, for the catalytic decomposition of methane (CDM), exhibiting the highest methane conversion (60 %), which is 1.4–2.1 times higher than the Ni-based classic-structured mesoporous siliceous supported catalysts, such as SBA15-S and MCM41-S. In particular, the H2 yield (62 %) of the Ni/MCF-S catalyst was 1.40 and 2.38 times higher than that of the Ni/SBA15-S and Ni/MCM41-S catalysts, respectively. To understand the observed differences, a detailed characterization of the physicochemical properties of these materials was conducted. The results revealed that the macro/mesopores size (4–60 nm) and bimodal sinusoidal pore geometry of MCF-S, played a critical role in enhancing Ni particle dispersion, resulting in the highest active Ni metal surface area (7.66 m2/gcat) and contributing to the improved catalytic activity of Ni catalysts in methane cracking.