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Co-based catalysts have shown great promise for propane dehydrogenation (PDH) reactions due to their merits of environmental friendliness and low cost. In this study, ordered mesoporous molecular sieve-supported CoO_x species (CoO_x/Al-SBA-15 catalyst) were prepared by one-step organometallic complexation. The catalysts show worm-like morphology with regular straight-through mesoporous pores and high external specific surface area. These typical features can substantially enhance the dispersion of CoO_x species and mass transfer of reactants and products. Compared with the conventional impregnation method, the 10CSOC (10 wt.% Co/Al-SBA-15 prepared by the organometallic complexation method) sample presents a smaller CoO_x size and higher Co²⁺/Co³⁺ ratio. When applied to PDH reaction, the 10CSOC delivers higher propane conversion and propylene selectivity. Under the optimal conditions (625 °C and 4500 h⁻¹), 10CSOC achieves high propane conversion (43%) and propylene selectivity (83%). This is attributed to the smaller and better dispersion of CoO_x nanoparticles, more suitable acid properties, and higher content of Co²⁺ species. This work paves the way for the rational design of high-performance catalysts for industrially important reactions.