Ionic　liquid　electrolytes　(ILEs)　are　promising　to　develop　high-safety　and　high-energy-density　lithium-metal　batteries　(LMBs).　Unfortunately,　ILEs　normally　face　the　challenge　of　sluggish　Li+　transport　due　to　increased　ions’　clustering　caused　by　Coulombic　interactions.　Here　a　type　of　anion-reinforced　solvating　ILEs　(ASILEs)　is　discovered,　which　reduce　ions’　clustering　by　enhancing　the　anion–cation　coordination　and　promoting　more　anions　to　enter　the　internal　solvation　sheath　of　Li+　to　address　this　concern.　The　designed　ASILEs,　incorporating　chlorinated　hydrocarbons　and　two　anions,　bis(fluorosulfonyl)　imide　(FSI−)　and　bis(trifluoromethanesulfonyl)　imide　(TFSI−),　aim　to　enhance　Li+　transport　ability,　stabilize　the　interface　of　the　high-nickel　cathode　material　(LiNi0.8Co0.1Mn0.1O2,　NCM811),　and　retain　fire-retardant　properties.　With　these　ASILEs,　the　Li/NCM811　cell　exhibits　high　initial　specific　capacity　(203　mAh　g−1　at　0.1　C),　outstanding　capacity　retention　(81.6%　over　500　cycles　at　1.0　C),　and　excellent　average　Coulombic　efficiency　(99.9%　over　500　cycles　at　1.0　C).　Furthermore,　an　Ah-level　Li/NCM811　pouch　cell　achieves　a　notable　energy　density　of　386 Wh　kg−1,　indicating　the　practical　feasibility　of　this　electrolyte.　This　research　offers　a　practical　solution　and　fundamental　guidance　for　the　rational　design　of　advanced　ILEs,　enabling　the　development　of　high-safety　and　high-energy-density　LMBs.　©　2024　Wiley-VCH　GmbH.