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A major challenge in the pursuit of higher‐energy‐density lithium batteries for carbon‐neutral‐mobility is electrolyte compatibility with a lithium metal electrode. This study demonstrates the robust and stable nature of acloso‐borate based gel polymer electrolyte (GPE), which enables outstanding electrochemical stability and capacity retention upon extensive cycling. The GPE developed herein has an ionic conductivity of 7.3 × 10⁻⁴ S cm⁻²at room temperature and stability over a wide temperature range from −35 to 80 °C with a high lithium transference number ( = 0.51). Multinuclear nuclear magnetic resonance and Fourier transform infrared are used to understand the solvation environment and interaction between the GPE components. Density functional theory calculations are leveraged to gain additional insight into the coordination environment and support spectroscopic interpretations. The GPE is also established to be a suitable electrolyte for extended cycling with four different active electrode materials when paired with a lithium metal electrode. The GPE can also be incorporated into a flexible battery that is capable of being cut and still functional. The incorporation of acloso‐borate into a gel polymer matrix represents a new direction for enhancing the electrochemical and physical properties of this class of materials.