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It is significant to improve the catalytic activity of TS-1 by increasing the content of framework titanium and enhancing the accessibility of active titanium sites. However, developing a simple and economical strategy for modulating the coordination environments and the spatial distribution of titanium species is still a challenge. Here, we constructed anatase-free TS-1 with abundant framework titanium species and Ti-rich surface by a simple two-step crystallization strategy. The effects of the crystallization temperature and time of the first stage on the properties of zeolite have been investigated in detail. The TS-1 with a Ti-rich surface showed a higher conversion of phenol and selectivity to dihydroxylbenzene in phenol hydroxylation reaction compared with traditional TS-1, and it still remained the superior catalytic performance after five cycles. The novel strategy will provide a new perspective for the construction of TS-1 with controllable active Ti species. [Display omitted] • The framework Ti content and the active Ti sites on the external surface of TS-1 were increased. • The temperature and time in the first stage have an important impact on the synthesis process. • The TS-1 zeolite prepared has good accessibility of active sites. • The novel strategy provides a new perspective for preparing other metal-doped zeolite with excellent catalytic activity. [ABSTRACT FROM AUTHOR]