Lithium-Metal Batteries In article number 2401957, Kim, Lee, Choi, and co-workers present a succinonitrile (SN)-rich electrolyte for lithium-metal batteries, demonstrating stable operation across a broad temperature range from −10°C to 45 °C. The SN-rich electrolyte facilitates the formation of a LiF-rich solid-electrolyte interphase and an N-rich cathode–electrolyte interface. Furthermore, the distinctive SN-based solvation structure reduces the electrolyte's freezing point and viscosity, thereby improving its bulk properties and overall electrochemical performance.