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In the cutting-edge era of wearable electronics,flexible lithium-ion batteries are considered more eye-catching.However,their applications are primarily limited by the low open-circuit voltage and energy density,which result from the irreversible intercalation of lithium ions into carbon-based current collectors.In this regard,we investigate to design a novel surface/interface strategy to obtain electrolyte-phobic carbon nanotubes and enhance the electrolyte repellence for the carbon-based current collector in the foldable lithium-ion battery.As a result,the assembled batteries exhibit a high open-circuit voltage of 4.04 V and energy density of~293 Wh kg-1 with excellent flexibility and stable cycle performance.Such outstanding results are ascribed to the electrolyte-phobic interfacial layer formed on the current collector,which restrains the direct contact between CNTs and lithium ions in the electrolyte.Therefore,this investigation not only demonstrates a practical solution to appreciably revamp the voltage and thereby energy density of flexible lithium-ions batteries,but more importantly offers valuable insights in modifying interface of carbon-based current collectors for high-performance energy storage devices.