Precisely　tuning　the　location　of　Al　atoms　in　zeolite　framework　that　plays　a　critical　role　in　determining　the　catalytic　performance　of　zeolite　based　catalysts　has　attracted　considerable　attention.　In　this　article,　we　present　an　organotemplate-free　approach　for　the　controllable　synthesis　of　ZSM-5　zeolite　with　a　high　content　of　Al　pairs　selectively　located　at　the　channel　intersections,　which　is　achieved　by　using　a　submolten　salt　(SMS)　depolymerized　rectorite　as　both　the　Al　source　and　heteropical　crystalline　seeds.　The　quasi　in-situ　characterizations　tracking　the　zeolite　crystallization　process　reveal　that　the　depolymerized　rectorite　with　abundant　oligomeric　aluminosilicate　species　and　Al–O-(Si–O)1,2-Al　sequences　plays　dual　roles　in　the　synthesis　of　ZSM-5　zeolite.　These　oligomeric　aluminosilicate　species　like　5-　and　6-membered　ring　structures　serve　as　the　crystalline　seeds　to　promote　the　zeolite　nucleation;　simultaneously,　the　Al–O-(Si–O)1,2-Al　sequences　are　in-situ　transformed　into　the　final　zeolite　framework　leading　to　the　generation　of　numerous　Al　pairs　selectively　located　at　the　channel　intersections.　Such　an　unusual　Al　distribution　endows　the　synthesized　ZSM-5　zeolite　with　excellent　catalytic　performance　in　methanol　to　aromatics　(MTA)　reaction.　Our　strategy　provides　a　sustainable　and　efficient　way　to　design　and　synthesize　high-performance　zeolites　with　special　framework　Al　distributions　for　catalytic　applications.　©　2020　Elsevier　Inc.