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A significant obstacle in the large‐scale applications of sodium borohydride (NaBH4) for hydrogen storage is its high cost. Herein, we report a new method to synthesize NaBH4 by ball milling hydrated sodium tetraborate (Na2B4O7 ⋅ 10H2O) with low‐cost Al or Al88Si12, instead of Na, Mg or Ca. An effective strategy is developed to facilitate mass transfer during the reaction by introducing NaH to enable...