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.　©　2019　American　Chemical　Society.