Praseodymium (Pr)-promoted MCM-41 catalyst was investigated for the catalytic decomposition of methyl mercaptan (CH₃SH). Various characterization techniques, such as X-ray diffraction (XRD), N₂ adsorption–desorption, temperature-programmed desorption of ammonia (NH₃-TPD) and carbon dioxide (CO₂-TPD), hydrogen temperature-programmed reduction (H₂-TPR), and X-ray photoelectron spectrometer (XPS), were carried out to analyze the physicochemical properties of material. XPS characterization results showed that praseodymium was presented on the modified catalyst in the form of praseodymium oxide species, which can react with coke deposit to prolong the catalytic stability until 120 h. Meanwhile, the strong acid sites were proved to be the main active center over the 10% Pr/MCM-41 catalyst by NH₃-TPD results during the catalytic elimination of methyl mercaptan. The possible reaction mechanism was proposed by analyzing the product distribution results. The final products were mainly small-molecule products, such as methane (CH₄) and hydrogen sulfide (H₂S). Dimethyl sulfide (CH₃SCH₃) was a reaction intermediate during the reaction. Therefore, this work contributes to the understanding of the reaction process of catalytic decomposition methyl mercaptan and the design of anti-carbon deposition catalysts.