We developed trimethyl phosphate (TMP)-based nonflammable electrolytes with a high TMP content exceeding 70% to increase the safety of lithium-ion cells with a graphite anode. TMP exhibits good oxidation stability and poor reduction stability at the graphite anode; therefore, we focused our efforts on suppressing TMP reduction decomposition at the graphite anode during charging. We selected a graphite material, named STG, with a surface partly coated by amorphous carbon particles to improve the TMP reduction stability. A new ternary mixed additive, 2 wt % vinylene carbonate +8 wt % vinyl ethylene carbonate +2 wt % cyclo hexane, was developed to exert a synergistic effect to improve the charge-discharge performance of the STG anode in TMP-based electrolytes. We further found that a high-concentration lithium bisperfluoroethylsulfonyl imide [LiN(SO2C2F5)(2)], of 2 mol dm(-3) was effective for suppressing TMP decomposition at the STG anode surface. Consequently, we were able to realize excellent cycling performance of an STG anode with over 70% TMP nonflammable electrolytes by applying the above approaches. This is the first report of such excellent performance of a graphite anode with high-content TMP-based nonflammable electrolytes. (c) 2005 The Electrochemical Society.