conductivity and interface issues in SSLBs are still two main difficulties to be overcome. Although high ionic conductivity of solid-state electrolytes (SSEs) has been achieved, the solid-solid interface issues severely impede the development of practical application in SSLBs, especially about interfaces in cathode materials. [4,5] In terms of the cathode/SSE interface, one main issue is poor physical contact. [6,7] It results in increased interface impedance and inefficient lithium-ion transport. After several cycles, volume expansion/ contraction of cathode materials will lead to physical delamination. [8,9] Another problem is the intrinsic electrochemical instability between the cathode/SSE interface, especially in SSLBs with sulfide solid electrolytes. [10] As a result, complex side reactions significantly reduce the interface compatibility, and the by-products formed after electrolyte degradation will greatly increase the impedance of batteries. [11,12] Apart from the cathode/SSE interface, the internal interface in the bulk cathode material is another bottleneck. [13] The gaps between particles in the bulk cathode of SSLBs fail to be connected as in the liquid electrolyte. Furthermore, the strength of point-to-point interfacial contact will also be more fragile under the volume change during cycling. [14] To achieve beneficial compatibility between the electrode/ SSE interface, artificial buffer layers were applied to optimize the interfaces in SSLBs. [15,16] They can provide steady interfaces with enhanced physical contacts and chemical/electrochemical stabilities. During the past several years, considerable related researches about coating-modified electrode/SSE interfaces have been reported, and great success has been achieved. [17,18] Although these methods can mitigate the interfacial problems to some extent, point-to-point contact between inside cathode particles is still remained to be solved. To overcome this phenomenon, buffer layers coating on individual cathode particles have been successively reported. [14,19] This core-shell structure makes use of the large contact area and numerous channels for rapid Li + transport, thus cathodes with higher Li + transport efficiency and lower interfacial impedance were fabricated. However, the sharp interfaces between SSE/bulk cathode and cathode/current collector still remain to be solved. The Solid-state lithium batteries (SSLBs) have attracted more attention due to their improved safety and high energy density. Although numerous solid-state electrolytes (SSEs) with high ionic conductivity have been frequently reported, poor solid-solid interfacial contact and interfacial chemical reactions around the cathode in SSLBs can hinder their practical application. Here, a gradient nanowire (NW) cathode is demonstrated for advanced interface engineering in SSLBs by a facile solvent evaporation process. In this unique gradient cathode membrane, one side surface with more ionic conductive polymer provides a smooth contact with SSE, while the other side surface with m...