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Li‐stuffed battery materials intrinsically have surface impurities, typically Li2CO3, which introduce severe kinetic barriers and electrochemical decay for a cycling battery. For energy‐dense solid‐state lithium batteries (SSLBs), mitigating detrimental Li2CO3 from both cathode and electrolyte materials is required, while the direct removal approaches hardly avoid Li2CO3 regeneration. Here, a decarbonization–fluorination...