A process coupling simultaneous production of hythane and carbon products via catalytic decomposition of methane (CDM) was carried out using iron catalysts dispersed on porous supports. The effect of different supports such as HZSM-5 zeolite, HBETA zeolite, and porous precipitated Al2O3 on catalytic decomposition of methane was investigated. The results showed that the ratio of hydrogen is around 10-30 vol% in the gaseous product which could be directly utilized as the clean fuel in the internal combustion engine. The solid carbon products with different morphologies such as open end or closed end carbon nanotubes (CNTs) were detected. The pore structure of the supports may have significant influence on the CNTs growth mechanism and production of hythane. (C) 2014 Elsevier Ltd. All rights reserved.