Hexagonally ordered rnesoporous MSU-S was assembled from nanoclustered zeolite seeds. The XRD and BET results verified that after treated in 10%H2O/N-2 atmosphere at 800 degrees C for 2 h, MSU-S still remained a well-ordered hexagonal structure due to rich acidic sites and excellent hydrothermal stability. A series of SmxMnyOz/MSU-S sorbents were prepared by a sol gel method. The desulfurization performances of the 55%Sm5Mn95/MSU-S sorbent were improved significantly due to high hydrothermal stability of MSU-S with high surface area as well as the synergistic effect between Mn and Sm2O3. The result of eight successive sulfurization/regeneration cycles of sorbent illustrated that high breakthrough sulfur capacity and endurable stability of 55%Sm5Mn95/MSU-S correlated closely with the existence of the framework 4-coordination aluminum (NH3-TPD, Al-27. MAS NMR) and high dispersion of Sm/Mn species on MSU-S (XRD, TPR) for H2S removal. HRTEM images and SAED patterns confirmed that fresh 55%Sm5Mn95/MSU-S existed in high ordered mesoporous structure and the nanosized Sm2O3 and Mn3O4 particles occurred in highly dispersive polycrystallites. The valence state of Mn species and the regeneration process of used sorbent were characterized by X-ray photoelectron spectroscopy (XPS) and TG/DSC. In addition, the effects of reaction temperature, feed composition and Sm/Mn atomic ratio in sorbents on desulfurization performance were investigated.