Argyrodite sulfide solid electrolytes (SSEs) have been attracting more concentration in ionic conductivity, crystal structure, and mechanical properties. Nevertheless, shortcomings of SSEs like poor air-vapor stability and interface reactions limit the wider application in batteries. Herein, a double-element ZnO substitution strategy is applied to enhancing Li5.5PS4.5Br1.5 Argyrodite electrolyte structure stability and property, Li5.5PS4.5Br1.5 electrolyte with a small amount of ZnO substitution to P and S. Li5.5+3xZnxP1-xOxS4.5-xBr1.5 solid electrolytes have achieved improved performance, interface composition also has changed, and crystal structure is becoming more stable. Specifically, LPSBr1.5-4%ZnO exhibits the most promising comprehensive properties, more expanded lithium pathway and crystal cell size, 2.25 mS cm-1 ionic conductivity at 25 °C, 65% electronic conductivity decline, and air stability enhancement. Moreover, LPSBr1.5-4%ZnO show decent lithium compatibility and dendrite suppression capability, LPSBr1.5-4%ZnO can continue cycling for more than 800h at 0.1 mA cm-2 in Li symmetric cell, and critical current density has reached 1.4 mA cm-2. More importantly, an all-solid-state battery (ASSB) with LPSBr1.5-4%ZnO electrolyte can cycle with 130 mAh g-1 capacity and more than 120 cycles in LiCoO2|SSE|In-Li cell. Our work might provide a strategy to promote structure stability and electrochemical durability, and how element substitution affects ionic transport pathway and crystal structure.