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In this report, a facile wet chemical method using acetonitrile combined with thermal annealing was used to prepare Li₂S‐P₂S₅(LPS) based glass‐ceramic electrolytes with (1 wt%, 3 wt%, and 5 wt% Ce₂S₃) and without Ce₂S₃doping. The crystal structure, ionic conductivity, and chemical stability of Li₇P₃S₁₁glass‐ceramic electrolytes were examined at varying temperatures (250–350°C). The results indicated that the highest ionic conductivity of 3.15 × 10⁻⁴S cm⁻¹for pure Li₇P₃S₁₁was observed at a temperature of 325°C. By incorporating 1 wt% Ce₂S₃and subjecting it to a heat treatment at 250°C, the glass ceramic electrolyte attained a remarkable ionic conductivity of 7.7 × 10⁻⁴(S cm⁻¹) at 25°C. Furthermore, it exhibited a stable and extensive electrochemical potential range, reaching up to 5 volts when compared to the Li/Li⁺reference electrode. By tuning the glass transition and crystallization temperature, cerium doping seems to make Li₇P₃S₁₁more chemically stable, compared to its original 70Li₂S‐30P₂S₅counterpart. According to Raman and X‐ray photoelectron spectroscopy analyses, cerium doping inhibits the decomposition of highly conductive P₂S₇^4‐(pyro‐thiophosphate) to PS₄³⁻and P₂S₆⁴⁻. Doped LPS has a greater crystallinity and more uniform microstructure than pure LPS, according to XRD, Raman spectroscopy, and scanning electron microscopy analysis. Consequently, Li₇P_2.9Ce_0.1S₁₁electrolyte shows great potential as a solid‐state electrolyte for constructing high‐performance sulfide‐based all‐solid‐state batteries.