ARTICLE This journal isThe deactivation pathways of a zeolite H-ZSM-5 catalyst, containing bentonite and α-Al2O3 as binder material, have been studied during the transformation of chloromethane into light olefins, which is considered as a possible step to valorize methane from natural gas. The reactions have been carried out in a fixed bed reactor, feeding pure chloromethane at 400, 425 and 450 °C; 1.5 bar and with a space-time of 5.4 (gcatalyst) h (molCH2) -1 during 255 min. The properties of the fresh and spent catalysts have been assessed by several techniques, such as N2 physisorption, adsorption/desorption of NH3, XPS and 29 Si NMR. Additional measurements of the spent catalysts have been performed to study the nature of the deactivating coke species: TG-TPO, SEM, FT-IR and UV-vis spectroscopies. With the results in hand, two deactivation mechanisms were proposed: irreversible dealumination at temperatures higher than 450 °C by HCl and reversible coke fouling, while coke formation results from the condensation of poly-alkylbenzenes, which are also intermediates for olefin production. The coke deposits grow in size with the addition of Cl to the carbonaceous structure.