Hybrid solid electrolytes (HSEs) with satisfactory ionic conductivities, good flexibilities, and ideal interface compatibilities are crucial for the development of allâsolidâstate lithiumâmetal batteries. However, Li dendrites and sluggish interfacial Li+ transfer dynamics between the Li metal and HSEs restrict practical applications. Herein, a facile strategy is proposed to promote homogeneous interfacial Li+ migration by modifying HSEs by using nitrogen plasma. N2 plasma not only decreases the crystallinity and glass transition temperature of HSE but also inâsitu generates an ultraâstable and conductive Li3N layer on the HSE surface. This conductive layer promotes interfacial Li+ migration and favorable wettability, thus effectively improving Li+ transfer dynamics and homogeneous deposition. Therefore, a HSE modified by N2 plasma for 10 s exhibits a low interfacial impedance of 26.5 Ω cmâ2 and a high Li+ conductivity of 7.35 Ă 10â5 S cmâ1 at 30 °C. Moreover, a symmetric Li|HSE|Li battery exhibits a stable plating/stripping capability without Li dendrite growth at a current density of 0.1 mA cmâ2 during continuous operation over 1000 h. In addition, an allâsolidâstate Li|HSE|LiFePO4 battery exhibits an initial specific capacity of 145.0 mAh gâ1 at 1 C with a high capacity retention of 92.4% (134.0 mAh gâ1) after 140 cycles.