Hydrogen technology is a viable alternative to carbon-based energy sources. However, the widespread use of hydrogen energy is limited by its low volumetric energy density, complex supply chain, and difficulties related to hydrogen storage. This study investigates the influence of Pt-supported graphene additives on hydrogen formation and decomposition of methylcyclohexane (MCH), which is a potential hydrogen carrier, by conducting high-pressure liquid flow reactor experiments and reactive force-field molecular dynamics simulations. This investigation represents a notable improvement in the MCH decomposition and hydrogen generation efficiencies through enhanced catalytic dehydrogenation facilitated by Pt-decorated functionalized graphene sheets (Pt@FGSs). Experimental results indicate that under fixed reaction conditions, the bicomposite structure of the Pt@FGSs at a loading concentration of 50 ppmw reduces the dehydrogenation energy and increases the conversion rate by up to 45%. The yields of products such as hydrogen and low-carbon species are also significantly improved. Notably, hydrogen formation is enhanced by a factor of approximately 2, demonstrating the effectiveness of Pt@FGSs in facilitating fuel decomposition and promoting hydrogen production. In addition, reactive force-field molecular dynamics simulations elucidate possible enhancement mechanisms, in which Pt nanoparticles attach to FGSs and catalyze the dehydrogenation of MCH and its derivatives. The production of a higher amount of the produced hydrogen is evidenced by the desorption of H atoms attached to the Pt surface. This study provides valuable insights that can accelerate the transition towards sustainable and effective decarbonization strategies using MCH as a hydrogen carrier.