The new hybrid of graphenated carbon nanotubes (g-CNTs) was superior to either CNTs or graphene.. Mesoporous 3D cubic Ni/KIT-6 were synthesized hydrothermally through organic template route and then were used as catalytic template for the production of g-CNTs using acetylene as a carbon precursor by chemical vapor deposition (CVD) method. The deposited new hybrid carbon materials were purified and analyzed by various physico-chemical techniques such as XRD, TGA, SEM, TEM and Raman spectroscopy techniques. The graphitization of CNTs was confirmed by TGA and HRTEM studies. Thermal stability, surface morphology, and structural morphology of these materials were revealed by TGA, SEM and TEM analysis, respectively. Moreover, the tailored mesoporous Ni/KIT-6 molecular sieves were found to possess better quality and massive quantity of g-CNTs produced compared to other catalytic template route. (C) 2013 Elsevier Ltd. All rights reserved.