Efficient storage and transportation of hydrogen are the bottlenecks limiting the development of hydrogen economy. One effective way to solve this problem is to store hydrogen in liquid organic hydrogen carriers, such as methanol, which can be released from the organic hydrogen carriers as H2 gas after catalyzed reforming process. The main challenge during this procedure is the development of catalysts capable of executing such a decomposition process. In this work, a novel organometallic compound RuHI(CO)(i⁃Pr⁃Imidazole)(PPh3)2 was synthesized and explored its catalytic applications for hydrogen production during aqueous methanol reforming. The compound was characterized by elemental analysis, infrared spectroscopy, and single⁃crystal X⁃ray diffraction for determining its cystalline structure. The results indicate that the organometallic compound, shows mononuclear structure with six⁃coordinated ruthenium ion in its network, forming the twisted octahedral configuration in the compound. It has been found that reaction conditions such as temperature, the type of alkali, the volume ratio of MeOH and H2O, have profound effects on the reaction efficiencies. Under optimized conditions (110 ℃, 8 mol/L KOH, V(MeOH)/V(H2O)=9∶1),4 μmol the catalyst produces a accumulated TON of 7 9:1 after a 14-day reaction.