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The ideal solid-state electrolyte must have exceptional chemical and electrochemical stability, high ionic conductivity, lower interfacial resistance and high active material utilization. Inspired by discovering new lithium thiophosphate superionic conductors for all-solid-state Li/S batteries (ASSLSBs), we designed and explored the local structure of Li_6.95Zr_0.05P_2.9S_10.8O_0.1I_0.4 (LZPSOI) solid-state electrolyte, which owns a high ionic conductivity of 3.01 mS cm⁻¹ with improved air-stability at RT. The structure–property correlation behavior of the chemical stability of LZPSOI electrolyte was sequentially premeditated by a combination of ex-situ XRD, MAS-NMR, XPS and SEM. A mechanistically driven approach has been extensively evaluated that the chemical stability of Li₇P₃S₁₁ could be enhanced via oxide doping, in which S^2- was partly replaced by O^2– in conductive structural units to yield POS₃^3- and P₂OS₆⁴ …