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Summary: Using quasi-solid electrolytes (QSEs) can make lithium metal batteries (LMBs) considerably safer. However, formulating QSEs with rate capabilities rivaling those of liquid electrolytes is extremely difficult. Herein, we develop a QSE characterized by safety, high conductivity above 2 × 10−3 S cm−1, and high lithium-ion transference number (tLi+) above 0.8. Computations and experiments reveal that these characteristics are achieved by adjusting the Li+ solvation through a weak interaction with the polymer skeleton and strong coordination with NO3−. The further inclusion of fluoroethylene carbonate leads to the formation of a Li3N- and LiF-rich solid electrolyte interphase on the lithium metal. Consequently, QSE-based LMBs are capable of fast charging and high-power density, as well as stable and long cycling. By adjusting Li+ solvation and lithium metal stability, this work rationally develops QSEs for fast-charging LMBs.