Liquid organic hydrogen carrier systems (LOHCs) are an efficient approach for storing hydrogen in organic molecules. Catalytic hydrogenation makes it possible to safely store and efficiently store and transport hydrogen. By dehydrogenation, hydrogen can be released. However, high temperatures are required for the dehydrogenation reaction, which reduces process efficiency and decomposes organic substances as a side reaction, limiting reuse. In this study, a low-temperature dehydrogenation reaction was performed using 1-methylindole (NMID)/Octahydro-1-methylindole (8H-NMID) as a heterocyclic LOHC compound containing a nitrogen atom in a ring structure. As a strategy to enhance the Pd-catalyzed dehydrogenation performance, MoOx was added to control the electronic structure of Pd. The addition of a small amount of MoOx to the Pd/Al2O3catalyst improved the Pd dispersion due to hydrogen spillover, resulting in a 1.52-fold increase in dehydrogenation activity compared to the original Pd/Al2O3.