High-voltage spinel manganese oxide LiNi0.5Mn1.5O4 (LNMO) that possesses high energy densities, high thermal and electrochemical stabilities, good operating safeties, low costs, and good rate performance has been well recognized to have great potential for power batteries. Despite these merits, unqualified electrolytes are still a big obstacle toward mass production of LNMO-based lithium-ion batteries (LIBs). To address this obstacle, solid polymer electrolytes (SPEs) have been increasingly considered as promising candidates thus far. Here, we mainly discuss the inherent advantages and ideal requirements of SPEs coupling with LNMO cathodes and then systematically review the recent advances of SPEs from the perspective of structure–performance relationships for the first time. Finally, prospects and challenges of the SPE systems are also discussed. This Review aims to guide rational structure design and future development of state-of-the-art SPEs with high anodic stabilities, boosting the practical applications of high-voltage LNMO cathode-based LIBs.

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High voltage spinel manganese oxide LiNi0.5Mn1.5O4 (LNMO) cathodes are promising for practical applications owing to several strengths including high working voltages, excellent operating safety, low costs, and so on. However, LNMO-based lithium–ion batteries (LIBs) fade rapidly mainly owing to unqualified electrolytes, hence becoming a big obstacle toward practical applications. To tackle this roadblock, substantial progress has been made thus far, and yet challenges still remain, while rare reviews have systematically discussed the status quo and future development of electrolyte optimization coupling with LNMO cathodes. Here, we discuss cycling degradation mechanisms at the cathode/electrolyte interface and ideal requirements of electrolytes for LNMO cathode-equipped LIBs, as well as review the recent advance of electrolyte optimization for LNMO cathode-equipped LIBs in detail. And then, the perspectives regarding the future research opportunities in developing state-of-the-art electrolytes are also presented. The authors hope to shed light on the rational optimization of advanced organic electrolytes in order to boost the large-scale practical applications of high voltage LNMO cathode-based LIBs.