A facile approach to fabricate a self-standing GPE for fl exible lithium-ion batteries is demonstrated using a UV-cured trivalent/monovalent acrylate polymer matrix and a liquid electrolyte. The polymer matrix is successfully synthesized with the co-presence of the liquid electrolyte by UV polymerization of ETPTA, which has trivalent vinyl groups, and EGMEA, which contains monovalent vinyl groups, with the ETPTA/EGMEA ratio fi xed at 90/10 (wt%/wt%). The ETPTA/EGMEA matrix shows a lower T g than the ETPTA matrix alone, which helps improve the mechanical fl exibility and ionic transport of the resulting GPE. These features of the ETPTA/EGMEA-based GPE, together with its superior interfacial compatibility towards electrodes, play crucial roles in obtaining a better cell performance compared to the ETPTA-based GPE. 0 4 8 1 2 1 6 0 20 40 60 80 100 120 140 160 Capacity (mAh g -1 ) Cycle number E-GPE M-GPE (E-GPE) σ = 1.30 S cm -1 (M-GPE) σ = 1.66 S cm -1properties is diffi cult to avoid. In addition, liquid electrolytes also tend to provoke undesired interfacial reactions of the GPEs with the electrodes during cell operation. [10][11][12] This may induce vigorous proliferation of a resistive layer on the electrodes, which hinders ionic transport at the interface of the GPE and liquid electrolyte. These drawbacks of GPEs pose a formidable challenge in their successful application to lithium-ion batteries. Hence, the realization of advanced GPEs with well-tuned mechanical/electrochemical properties is urgently needed.To this end, we have developed a new, self-standing GPE for a design-fl exible lithium-ion battery by exploiting a UV-cured trivalent/monovalent acrylate polymer matrix and a liquid electrolyte (1 M LiPF 6 in ethylene carbonate (EC)/diethyl carbonate (DEC) = 1/1 v/v). The UV irradiation of vinyl monomers is a well-established, free-radical photopolymerization technique. UV polymerization can be conducted without the use of a solvent and requires a very short exposure time of less than a few minutes, thereby providing a facile and effective synthesis route for the preparation of polymers. [13][14][15][16] The UV-polymerizable trivalent/monovalent acrylate mixture employed in the present study was composed of