Solid-state polymer electrolytes (SPEs) with flexibility, easy processability, and low cost have been regarded as promising alternatives for conventional liquid electrolytes in next-generation high-safety lithium metal batteries. However, SPEs generally suffer poor strength to block Li dendrite growth during the charge/discharge process, which severely limits their wide practical applications. Here, a rational design of 3D cross-linked network asymmetric SPE modified with a metal-organic framework (MOF) layer on one side is proposed and prepared through an in-situ polymerization process. In such unique asymmetric SPEs, the nanoscale MOF layer acts as a shield that effectively suppresses the growth of Li dendrites and regulates the uniform Li + transport, and the polymer electrolyte can be scattered in the whole cell to endow the smooth transmission of Li +. As a result, the asymmetric SPE exhibits high ionic conductivity, wide electrochemical window, high thermal stability and safety, which endows the Li/Li symmetrical cell with outstanding cyclic stability (operate well over 800 h at a current density of 0.1 mA cm −2 for the capacity of 0.1 mAh cm −2).