Controllable　synthesis　of　hierarchical　zeolites　from　natural　aluminosilicate　minerals　is　considered　an　efficient　and　eco-friendly　approach　for　the　production　of　high-performance　zeolites,　but　its　synthesis　mechanism　is　still　obscure.　Herein,　we　take　the　synthesis　of　a　single-crystalline　hierarchical　NaA　zeolite　using　submolten　salt　depolymerized　kaolin　(SMS-K)　as　the　sole　source　of　silicon　and　aluminum　via　a　mesoscale　reorganization　strategy　as　an　example　to　elucidate　the　reorganization　process.　Comprehensive　morphological　and　structural　analyses　reveal　that　sodium-rich　voids　in　SMS-K　facilitate　concurrent　assembly　both　within　the　interior　and　at　the　interface　of　the　amorphous　gel,　leading　to　the　formation　of　numerous　nanoparticles　with　short-range　order　which　assemble　into　single-crystal　nanocube　NaA　zeolites　with　intracrystalline　mesopores.　By　harnessing　confinement　effects,　SMS-K　modulates　the　growth　of　nanoparticle　sizes　and　enhances　the　intimate　interconnection　of　nanocubes,　thereby　yielding　NaA　zeolite　aggregates　that　exhibit　hierarchical　porosity,　encompassing　micro-,　meso-,　and　macropores.　This　study　offers　the　potential　for　designing　and　precisely　controlling　the　fabrication　of　hierarchical　zeolites　derived　from　natural　minerals.　©　2024　American　Chemical　Society.