Mesoporous alumina (MA) materials with outstanding textural properties have been synthesized by a facile approach, and were evaluated as supports of Pt-based catalyst for methylcyclohexane dehydrogenation. At 300 °C, the resultant catalyst demonstrates a much higher activity with a maximum hydrogen evolution rate of 2081 mmol/gPt/min in comparison with the state-of-the-art alumina supported Pt catalysts. Interestingly, even after a long-time reaction of 100 h or regeneration, more than 80% of original activity was still maintained. The superior catalytic performance of the obtained catalyst is associated with the high specific surface area and large mesoporous size of support MA, thus benefiting the increase in the number of Pt active sites and efficiently inhibiting the formation of coke deposition during the reaction. Our contribution has provided a rational design strategy for highly efficient and stable dehydrogenation catalysts, which is a key for the utilization of methylcyclohexane-toluene system in hydrogen storage technology. Display omitted •A confined hydrolysis-condensation approach.•Mesoporous alumina with excellent textural properties.•Pt-based catalyst with highly homogenous dispersion of Pt.•Improved catalytic performance for dehydrogenation of methylcyclohexane at low temperature.