Advancement of all-solid-state lithium-ion (Li⁺) batteries (ASSLIBs) has been hindered by the large interfacial resistance mainly originating from interfacial reactions between oxide cathodes and solid-state sulfide electrolytes (SEs). To suppress the interfacial reactions, an interfacial coating layer between cathodes and SEs is indispensable. However, the kinetics of interfacial Li⁺ transport across the coating layer has not been well understood yet. Herein, we tune the interfacial ionic conductivity of the coating layer LiNb_0.5Ta_0.5O₃ (LNTO) by manipulating post-annealing temperature. It is found that the interfacial ionic conductivity determines interfacial Li⁺ transport kinetics and enhancing the interfacial ionic conductivity can significantly boost the electrochemical performance of SE-based ASSLIBs. A representative cathode LiNi_0.5Mn_0.3Co_0.2O₂ coated by LNTO with the highest interfacial ionic conductivity exhibits a high initial capacity of 152 mAh.g^-1 at 0.1 C and 107.5 mAh.g^-1 at 1 C. This work highlights the importance of increasing interfacial ionic conductivity for high-performance SE-based ASSLIBs.

全固态锂离子（Li ⁺）电池（ASSLIB）的发展已受到主要来自氧化物阴极和固态硫化物电解质（SEs）之间的界面反应的大界面电阻的阻碍。为了抑制界面反应，在阴极和SE之间的界面涂层是必不可少的。但是，界面Li ⁺跨涂层传输的动力学尚未得到很好的理解。本文中，我们通过控制后退火温度来调整涂层LiNb _0.5 Ta _0.5 O ₃（LNTO）的界面离子电导率。发现界面离子电导率决定了界面Li ⁺传输动力学和增强界面离子电导率可以显着提高基于SE的ASSLIBs的电化学性能。代表性的阴极的LiNi _0.5锰_0.3钴_0.2 ø _2个具有最高的界面的离子传导性的展品152 mAh.g的高的初始容量通过涂覆LNTO ^-1以0.1C和107.5 mAh.g ^-1在1℃。该工作亮点对于基于SE的高性能ASSLIB，提高界面离子电导率的重要性。