Epoxidation catalytic technology is important for preparing organic chemical raw materials and fine chemical products. But it has drawbacks such as low catalytic efficiency and serious pollution problem. The key to realize sustainable energy development is to develop green epoxidation catalytic techniques. Selective oxidation over titanosilicate zeolite TS-1 is the key to achieve green epoxidation process. Aiming at solving the intracrystalline diffusion limitations in microporous zeolites caused by their relatively small micropores, this paper focuses on design and synthesis of hierarchically mesoporous zeolite TS-1 single crystals, investigation and development of the synthesis methods, and the influence of hierarchically meso-microporous hierarchy on the catalytic epoxidation of allyl chloride performances. Compared with microporous zeolite TS-1, the hierarchically mesoporous zeolite TS-1 has better catalytic activity.