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This work presents a facile synthesis approach for core–shell structured Li₂S nanoparticles with Li₂S as the core and Li₃PS₄ as the shell. This material functions as lithium superionic sulfide (LSS) cathode for long-lasting, energy-efficient lithium–sulfur (Li–S) batteries. The LSS has an ionic conductivity of 10^–7 S cm^–1 at 25 °C, which is 6 orders of magnitude higher than that of bulk Li₂S (∼10^–13 S cm^–1). The high lithium-ion conductivity of LSS imparts an excellent cycling performance to all-solid Li–S batteries, which also promises safe cycling of high-energy batteries with metallic lithium anodes.