LiNO3 is recognized as an effective additive, forming a dense, nitrogen-rich solid electrolyte interphase (SEI) on lithium's surface, which safeguards it from parasitic reactions. However, its use is limited due to the poor solubility in carbonate electrolytes. Herein, we introduce a bilayer separator designed to release LiNO3 sustainably. This continual release not only alters the chemistry of the SEI but also replenishes the additives that are depleted during battery cycling, thereby enhancing the durability of the modified interphase. This strategy effectively curtails Li dendrite formation, significantly enhancing the longevity of Li|LiFePO4 batteries, evidenced by an impressive 85% capacity retention after 800 cycles. This research offers a compelling remedy to the longstanding challenge of incorporating LiNO3 in carbonate electrolytes.