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A polymer electrolyte with a particular molecular architecture plays a critical role in the improvement of the performances of both a polymer electrolyte and a battery device. Here, we present the design and synthesis of a sp3‐boron‐based single‐ion polymer electrolyte (SIPE), lithium poly(bisphenol AF borate) (LiPFB), by using partially aromatic bisphenol AF as a linker. As a result of the torsional, flexible, and strong electron‐withdrawing properties of the bistrifluoromethyl methylene group (−C(CF3)2−), the prepared poly(vinylidene fluoride‐co‐hexafluoropropene (PVDF‐HFP)/LiPFB membrane displays an enhanced ionic conductivity and a remarkable compatibility with electrodes compared to that of the PVDF‐HFP/lithium poly(4,4′‐biphenol borate) membrane, in which a linear and fully aromatic 4,4′‐biphenol is used as a linker. Consequently, an excellent battery performance both at room temperature and high charge/discharge rates was demonstrated. This study underscores the fundamental importance of the molecular structure of SIPE materials in battery performance enhancement and suggests ways to design new SIPE materials to enhance battery devices with improved electrochemical performance.