[Objective] The aim was to explore the optimal conditions for the catalytic synthesis of geranyl propionate. [Method] The synthesis of mesoporous molecular sieves Al-MCM-41 was carried out in an open-vessel. The mesoporous structure of as-synthesized Al-MCM-41 was characterized by X-ray diffraction (XRD) pattern, Fourier transform infrared (FT-IR) spectrum, NH3-Temperature Programmed Desorption (TPD), and N2 adsorption-desorption isotherms. The catalytic performances of Al-MCM-41 for the synthesis of geranyl propionate (GP) with geraniol and propionic acid as reagents also were investigated. [Result] The as-synthesized Al-MCM-41 possesses typical hexagonal mesoporous structure with high long-range order and crystalline degree. Based on the systematic investigation of reaction time, temperature, amount ratio of reagents and regeneration of catalyst, the optimum reaction conditions were obtained with molar ratio of geraniol to propionic acid of 1.0∶1.5, reaction temperature of 120 ℃ and reaction time of 8 h. The high GP selectivity of 70.01% with geraniol conversion of 40.01% was achieved under above optimum conditions. The catalyst inactivation can be observed after five catalytic cycles. The regeneration of inactivated catalyst with high activity and selectivity can be achieved by calcination treatment to remove the carbon deposition, which covers the acid site of catalyst. [Conclusion] The optimal conditions for the synthesis of geranyl propionate were obtained.