Despite being an effective flame retardant, trimethyl phosphate (TMP a )i sg enerally considered as an unqualified solvent for fabricating electrolytes used in graphite (Gr)-based lithium-ion batteries as it readily leads to Gr exfoliation and cell failure.I nt his work, by adopting the unique solvation structure of localized high-concentration electrolyte (LHCE) to TMP a and tuning the composition of the solvation sheaths via electrolyte additives,excellent electrochemical performance can be achieved with TMP a -based electrolytes in Gr k Li-Ni 0.8 Mn 0.1 Co 0.1 O 2 cells.After 500 charge/discharge cycles within the voltage range of 2.5-4.4 V, the batteries containing the TMP a -based LHCE with ap roper additive can achieve ac apacity retention of 85.4 %, being significantly higher than cells using aL iPF 6 -organocarbonates baseline electrolyte (75.2 %). Meanwhile,d ue to the flame retarding effect of TMP a ,T MP a -based LHCEs exhibit significantly reduced flammability compared with the conventional LiPF 6 -organocarbonates electrolyte.