“…As an alternative to traditional flammable and highly chemically active liquid electrolytes, solid electrolytes (containing inorganic solid electrolytes, ISEs, and solid polymer electrolytes, SPEs) have been extensively investigated to improve the safety of next-generation lithium-based batteries. − Among them, SPEs have remarkable advantages over ISEs, such as tailorable synthesis, adjustable specific strength, scalable production, and excellent compatibility with rigid electrodes. − Although significant progress has been made for SPEs, the growth of lithium dendrites remains a primary cause of the rapid capacity decay in lithium metal batteries. Since the discovery by Monroe and Newman that lithium dendrites can be effectively suppressed when the elastic modulus of solid electrolytes is twice that of lithium metal, rigid artificial protective layers have been developed to mitigate the growth of lithium dendrites. − Nevertheless, the interfacial contact between rigid solid materials results in significant impedance and impacts the cycling performance of secondary batteries . Fortunately, it has recently been discovered that the utilization of flexible polymer electrolytes can significantly enhance the performance of lithium metal anodes (LMAs) by accommodating their volume fluctuation during deposition/dissolution. − For example, Nishikawa et al reported tough and stretchable gel polymer electrolytes (GPEs) possessing strong interchain hydrogen bonds in the presence of high concentrations of lithium salts .…”