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Mesoporous molecular sieve SBA-15 was successfully modified with 3-aminopropyltriethoxysilane (APTES) and 3-glycidyloxypropyltrimethoxysilane (GPTMS). The functionalized SBA-15 were characterized by small-angle X-ray (SAXRD), thermogravimetric analysis (TG), N2 adsorption, and Fourier transformed infrared spectrum (FT-IR). APTES functionalized SBA-15 (named SBA-15-A) and GPTMS functionalized SBA-15 (named SBA-15-G) were used to immobilize myoglobin (Mb). The loading amounts of Mb by SBA-15-A and SBA-15-G were 511.2 and 547.8 mg/g, respectively, whereas only 359.6 mg/g was achieved by SBA-15. Mb/SBA-15-G and Mb/SBA-15-A demonstrated better reusability than SBA-15, retaining 84.6% and 82.7% of the initial activity after repeated use seven times. The Mb/SBA-15-A and Mb/SBA-15-G also exhibited improved thermal stability and storage stability.