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In this work, nickel metal supported on different supports (SiO2, Al2O3, ZSM-5) were prepared by spraying nickel nitrate on the supports and calcined at 873 K. Then, they were characterized by XRD, XRF, N2 adsorption–desorption, NH3-TPD, MCH-TPD, H2-TPR, and pyridine-FTIR, and tested as catalysts for the dehydrogenation aromatization and isomerization of methylcyclohexane (MCH) under the conditions of S-Zorb catalytic adsorption desulfurization (T = 673 K, P = 1.5 MPa, WHSV = 5 h−1). The H2-TPR results showed that the interaction of NiO with support decreased in the order of NiO/ZSM-5-Fe < NiO/ZSM-5 < NiO/Al2O3 < NiO/SiO2. The decrease of the interaction appeared to facilitate the reduction of Ni and therefore to promote the dehydrogenation aromatization of MCH.It was found that a direct correlation existed between the gasoline components yields, cracking activity and the total number of different supports acid sites measured by NH3-TPD tests. Higher total acidity of ZSM-5 resulted in gasoline loss because of higher cracking activity of MCH. The number of total acid sites of NiO/ZSM-5-Fe decreased and the medium strong Brönsted acid sites necessary for MCH isomerization increased after the modification of ZSM-5 by iron metal. So, NiO/ZSM-5-Fe exhibited enhanced MCH conversion, aromatic and isomerization yields when compared to NiO/ZSM-5 and other Ni-based catalysts. This study shows that NiO/ZSM-5-Fe catalyst may be possible to be integrated into the S-Zorb system achieving the recovery of the octane number of gasoline. Keywords: Modified ZSM-5, Methylcyclohexane, Aromatization, Octane number