The　safety　and　cycle　stability　of　lithium　metal　batteries　(LMBs)　under　conditions　of　high　cut-off　voltage　and　fast　charging　put　forward　higher　requirements　for　electrolytes.　Here,　a　sulfonate-based　deep　eutectic　electrolyte　(DEE)　resulting　from　the　eutectic　effect　between　solid　sultone　and　lithium　bis(trifluoromethanesulfonyl)imide　without　any　other　additives　is　reported.　The　intermolecular　coordination　effect　triggers　this　eutectic　phenomenon,　as　evidenced　with　nuclear　magnetic　resonance,　and　thus　the　electrochemical　behavior　of　the　DEE　can　be　controlled　by　jointly　regulating　the　coordination　effects　of　FH　and　LiO　intermolecular　interactions.　The　DEE　with　a　properly　coordinated　environment　of　Li+　presents　a　low　motion　barrier　and　a　high　transport　rate　of　localized　Li+,　leading　to　a　10　C　fast-charging　LiFePO4||Li　battery　with　a　capacity　retention　of　95.1%　after　500　cycles.　Meanwhile,　the　strengthened　alpha-HF　coordination　broadens　the　electrochemical　stability　window　of　the　DEE,　thus　enabling　the　cycle　stability　of　high-capacity　and　high-voltage　cathode　materials　in　LMBs,　e.g.,　a　cycle　stability　at　4.5　V　in　the　LiNi0.88Co0.07Mn0.05O2||Li　battery　with　a　capacity　retention　of　81.0%　after　500　cycles,　and　an　excellent　compatibility　in　4.5　V　LiCoO2||Li　and　4.8　V　Li1.13Mn0.517Ni0.256Co0.097O2||Li　batteries.　The　practical　applicability　of　the　carefully　designed　DEE　is　underscored　through　successful　implementation　in　pouch　cells.