A novel technique for designing a robust solid electrolyte interface (SEI) on the negative electrodes of lithium-ion batteries has been developed using a silane coating. Two silane compounds, 3,3,3-trifluoropropyltrimethoxysilane (TFPTMS) and dimethoxybis(2-(2-(2-mothoxyethoxy)ethoxy)ethoxy)silane (1ND3(MeO)), have been investigated with respect to improving the capacity retention of lithium manganese oxide spinel/soft carbon cells. The impact of the silane coating on the soft carbon electrode will be attributed to (1) changes in surface functional groups, (2) compositional change of the SEI, and (3) changes in the kinetics of manganese deposition. The impact of the upper cutoff voltage on the capacity retention of the cell was also discussed.