The application of a chemical looping process to methane thermo-catalytic decomposition using activated carbon (AC) as a catalyst has been recognized as a promising technology for continuous high-purity H-2 production in a carbon constrained world. However, it usually needs an external heat supply for the endothermic decomposition reactions. By taking advantage of the chemical looping combustion (CLC) technology, this study proposed a deep regeneration approach using H2O and O-2 as regeneration agents to overcome the issues with maintaining catalytic activity and producing the heat needed for the endothermic reactions of H-2 production from methane. TG-DTA and bench scale fluidized bed experimental results indicate that a deep regeneration degree of 30% or above could completely reactivate the spent AC catalyst and simultaneously generate sufficient heat than required in the methane decomposition reaction. Characterization study implies that the deep regenerated AC catalyst could maintain its physical properties within a certain number of cycles. Based on the experimental results, the chemical looping methane thereto-catalytic decomposition process was further optimized and assessed by Aspen Plus (R) thermodynamic simulation. The results indicate that heat and mass balances could be attained, and the circulation of the AC catalyst with a temperature difference of 262 degrees C between the decomposer and the regenerator enabling the process to run autothermally. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.