This article reports a green strategy to synthesize Ti-ZSM-5 zeolites directly from a titanium-containing natural rectorite mineral, with particular emphasis on the transformation and crystallization behaviors of titanium species during the rectorite activation and the followed crystallization of the activated rectorites. The results show that when taking the alkali fusion and submolten salt activated rectorites as the starting materials, Ti-ZSM-5 zeolites with moderate acidity and superior hydroisomerization and aromatization performance are successfully obtained, in which part of Ti is isomorphically incorporated into the framework of the resulting ZSM-5 zeolites, whereas when taking the raw and thermally activated rectorites as the starting materials, ZSM-5 zeolites with TiO2 existing as impurities rather than as framework Ti atoms are obtained. This difference is attributed to the different chemical states of the titanium species in different activated rectorites. The approach reported here points to a green avenue to directly synthesize heteroatom-containing zeolites from natural clay minerals.