Summary In this study, hydrogen (H2) generation from the hydrolysis of sodium borohydride (NaBH4) catalyzed by bimetallic Palladium‐Ruthenium (PdRu) supported on multiwalled carbon nanotube‐graphene (MWCNT‐GNP) hybrid material is investigated. The effect of various parameters such as temperature, NaBH4 concentration, and catalyst loading and effect of base concentration are examined to observed optimum operating conditions. Experimental results show that the PdRu/MWCNT‐GNP bimetallic catalyst has high catalytic activity on NaBH4 hydrolysis reaction. It has been found that PdRu/MWCNT‐GNP catalyst shows low activation energy of 22.33 kJ/mol for hydrolysis reaction of NaBH4. The PdRu/MWCNT‐GNP catalyst also exhibits H2 generation rate of 79.2 mmol/min·gcat at 45°C. It shows good cycle stability in the catalyst reusability test and retained 89% of its initial catalytic activity after fifth use. The high catalytic activity of the PdRu/MWCNT‐GNP catalyst makes it promising in H2 generation from NaBH4 hydrolysis for commercial proton exchange membrane fuel cell (PEMFC) applications.