The application of high voltage cathode electrode materials is an effective way to increase the energy density of batteries. However, the development and design of a stable electrolyte at high voltages needs to be further addressed. Herein, we developed a non-flammable dual-salt deep eutectic solvent (DES) as a safe electrolyte containing LiTFSI, LiDFOB, and succinonitrile in different molar ratios. This non-flammable DES provides high ionic conductivity (4.23 mS cm−1) at 25 °C, high Li+ transference number (0.75), and wide electrochemical stability (>5.5 V). When using the designed DES electrolytes in high voltage LiCoO2||Li cells, superior electrochemical performance was achieved at cut-off voltages of 3.0–4.45 V and 3.0–4.6 V, even at a high current density of 2 C. This work offers an in-depth understanding of the critical role of dual-salts in DES and provides an approach to designing safe electrolytes for high voltage LiCoO2||Li cells.