The TS-1 microsphere was facilely prepared via a direct spray drying of the mixture containing the nanocrystal TS-1 and mother liquor. The calcined TS-1 zeolites possess a hollow structure and numerous intercrystalline mesopores, which may facilitate the diffusion properties. Au nanoparticles were loaded on TS-1 support by utilizing a deposition–precipitation process to prepare the Au/TS-1-M catalysts for propylene epoxidation in the presence of H2 and O2 conditions. The effects of the Ti and Au loadings on the structure, porosity, morphology, and catalytic performances of the Au/TS-1 catalysts have been investigated by various techniques. Under the optimized synthesis conditions (Si/Ti molar ratio = 57, 0.49 wt% Au), a propylene conversion of 6.1 % and a PO selectivity of 91.7 % were obtained on the Au/TS-1 catalyst. A PO formation rate of 186.8 gPO·kgcat.−1·h−1 was achieved at the 20th hour.