Safe fast‐charging lithium‐ion batteries (LIBs) can be achieved by using LiFePO4 electrode and optimized electrolyte for the rapid development of electric vehicles. However, conventional carbonate electrolyte suffers resistive solid electrolyte interphase (SEI) that hampering the fast‐charging for LIBs. Herein, a multiple additive strategy, the combination of 1,3,2‐Dioxathiolane 2,2‐dioxide (DTD) and lithium difluorophosphate (DFP), is proposed to optimize the electrode interface for graphite (Gr)/LiFePO4(LFP) pouch cells under fast‐charging. Combining DTD with DFP can significantly reduce the charge transfer resistance of anode and greatly extend the lifespan of cells with >2400 cycles at a 2 C rate, which is much better than that of baseline and single additive based electrolytes with <1000 cycles. Further mechanistic studies revealed that proper sulfurized and phosphatized species are involved in the SEI film, which stabilizes lithium carbonate in the middle of SEI to avoid being attacked by Lewis acids. Multiple additive strategies optimize the interfacial structure and provide valuable guidance for the development of safe fast‐charging engineering.
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