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We report an innovative cross-linked compositepolymer electrolyte (CPE) based on the garnet-type ceramicsuper Li+ion conductor, Li7La3Zr2O12(LLZO), that isencompassed in a supersoft poly(ethylene oxide)/tetraglymematrix. UV-induced, facile and solvent-free cross-linkingprocess ensuresflexible and self-standing CPEs, which arenonflammable and perfectly shape-retaining under thermal/mechanical stress. The CPEs exhibit high ionic conductivity,exceeding 0.1 mS cm?1at 20°C, suitable for ambient andsubambient temperature operation. Lab-scale lithium metalpolymer cells assembled with LiFePO4-based compositecathode and the optimized CPE deliver full capacity at lowcurrent rates and outstanding specific discharge capacity of 115mAh g?1at 1C rate and ambient temperature. Remarkably, the lithium metal cell can run for hundreds of galvanostatic cycles(>400) with low overpotential, limited fading, and excellent Coulombic efficiency (>99%), which postulates the practicalapplication of the newly developed CPEs as truly solid separating electrolytes in high-power energy storage technologies,assuring safety and performance in a wide range of operating conditions.