Several metal nanoparticle based catalysts have been synthesized for catalyzing the hydrogen production process by hydrolysis of methylamine-borane (MeAB). However, there was only one study that catalyzes the producing of hydrogen via the methanolysis of MeAB, and it was carried out by our research group. For this reason, in this work, a new catalyst system entitled by single-walled carbon nanotube (SWCNT) supported bimetallic platinum-ruthenium nanoparticles were developed and called as PtRu@SWCNT. These NPs were characterized by several techniques (XRD, XPS, Raman, and TEM), and they were performed for the methanolysis of MeAB with high catalytic activity. The prepared PtRu@SWCNT NPs were also tested in the methanolysis of MeAB at different parameters including different temperatures, catalyst and substrate concentrations, and reusability performance. Experimental results revealed that the new PtRu@SWCNT NPs had excellent catalytic activity and reusability for removing of hydrogen from the methanolysis of MeAB at ambient conditions. According to the obtained data, the turnover frequency is 136.25 mole H-2/mole PtRu x min, and the activation energy (Ea) is 17.29 kJ/mole. More than 99% of conversion was observed at room temperature.