Catalytic decomposition of natural gas has been opted as an alternative route for hydrogen production. Nickel- and Cobalt-based bimetallic catalysts over alumina support were prepared by the co-precipitation method for the investigation of hydrogen production via catalytic decomposition of methane. The effect of different important parameters such as reaction temperature, gas hourly space velocity (GHSV) and metal loading were studied. The catalytic activity and stability results revealed that the catalyst having 25 wt.% each of Ni and Co (25NCA) exhibited the best performance among all tested catalysts. The textural and morphological nature of the calcined and spent catalysts were examined using different characterization techniques including BET, temperature-programmed reduction (TPR), X-ray diffraction (XRD), thermo-gravimetric analysis (TGA), scanning electron microscopy (SEM) and high resolution transmission electron microscopy (HR-TEM). Copyright (C) 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.