Li metal batteries (LMBs), owing to their high theoretical specific energy, are considered a crucial development direction for future high-energy-density battery systems. However, the high reactivity of the Li metal anode leads to extreme electrochemical and chemical instability at the interface with the electrolyte. This instability triggers detrimental effects, including Li dendrite growth, repeated cracking and reformation of the solid electrolyte interphase (SEI), and continuous irreversible consumption of both active Li and electrolyte. Therefore, designing high-performance electrolytes to precisely regulate interfacial chemistry has become one of the core strategies for advancing the practical application of LMBs. Significant progress has recently been made in stabilizing the Li metal–electrolyte interface (Li-electrolyte interface) through strategies including additives, weakly solvating electrolytes (WSEs), high-concentration/localized high-concentration electrolytes (HCEs/LHCEs), and novel molecular design. Nevertheless, these advanced strategies and their corresponding stabilization mechanisms have not yet been systematically organized. To address this gap, this review focuses on four core electrolyte design strategies and systematically summarizes their mechanisms for stabilizing the Li-electrolyte interface. Building on this foundation, it discusses the inherent limitations of individual electrolyte design strategies. It then focuses on the potential of synergistic electrolyte design to achieve a more electrochemically stable Li-electrolyte interface. Finally, it proposes future research directions requiring key focus for existing electrolyte design strategies.

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