In this study, the LaNi5 metal hydride is used as a catalyst for the hydrogenation of toluene producing methylcylohexane (MCH) in a Liquid Organic Hydrogen Carrier (LOHC) application. Hydrogenation reactions are conducted at temperatures of 348, 363, 373, 383, and 393 K under a hydrogen pressure of 3 MPa. Nuclear Magnetic Resonance (NMR) and Gas Chromatography (GC) analyses reveal a conversion rate of 99.9 % at temperatures higher than 383 K. Pressure-Composition-Temperature (PCT) measurements indicate that, at this temperature and pressure, LaNi5 is in its dehydrogenated state, assisting the toluene hydrogenation by supplying absorbed hydrogen stored within the hydride back to toluene. On the other hand, even under conditions where hydrogen cannot not be desorbed from LaNi5, a moderate conversion of toluene to MCH is observed, indicating the role of elemental Ni on the surface of LaNi5. These finding highlight the dual functionality of LaNi5 as both a hydrogen storage material and an effective catalyst for LOHC hydrogenation.