The solid polymer electrolyte(SPE)is one of the most promising candidates for building solid lithium bat-teries with high energy density and safety due to its advantages of flexibility and light-weight.However,the conventional monolayered electrolytes usually exhibit unstable contacts with either high-voltage cathodes or Li-metal anodes during cell operation.Herein,heterogeneous dual-layered electrolyte mem-branes(HDEMs)consisting of the specific functional polymer matrixes united with the designed solid ceramic fillers are constructed to address the crucial issues of interfacial instability.The electrolyte layers composed of the high-conductivity and oxidation-resistance polyacrylonitrile(PAN)combined with Li0.33La0.557TiO3 nanofibers are in contact with the high-voltage cathodes,achieving the compatible inter-face between the cathodes and the electrolytes.Meanwhile,the electrolyte layers composed of the high-stability and dendrite-resistance polyethylene oxide(PEO)with Li6.4La3Zr1.4Ta0.6O12 nanoparticles are in contact with the Li-metal anodes,aiming to suppress the dendrite growth,as well as avoid the passiva-tion between the PAN and the Li-metal.Consequently,the solid LiNi0.6Co0.2Mn0.2O2||Li full cells based on the designed HDEMs show the good rate and cycling performance,i.e.the discharge capacity of 170.1 mAh g-1 with a capacity retention of 78.2%after 100 cycles at 0.1 C and 30℃.The results provide an effec-tive strategy to construct the heterogeneous electrolyte membranes with double-side stable electrode/-electrolyte interfaces for the high-voltage and dendrite-free solid lithium batteries.