The advanced electrolyte of liquid metal battery should have low melting point, low ionic solubility, low viscosity, high electric and thermal conductivities, and a suitable density between anode and cathode for declining the operating temperature and realizing the goal of saving‐energy. In this study, an excellent quaternary LiF−LiCl−LiBr−LiI (9.1 : 30.0 : 21.7 : 39.2) electrolyte is refined by using thermodynamic models to balance various properties of LiX (X=F, Cl, Br, I) and meet the requirement of advanced electrolyte of liquid metal battery. The refined properties of electrolyte correspond to 2.398 g/cm3 for density, 0.286 mol% for solubility, 4.486 Ohm−1 cm−1 for ionic conductivity, and 0.609 W m−1 for thermal conductivity. The measured melting point is 609.1 K, which is lower than the current operating temperature of 723 K for the lithium‐based liquid metal battery. The refined electrolyte consisted by quaternary halide molten‐salt provides important references for preparing the advanced liquid metal battery.