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Flexible energy devices with high energy density and long cycle life are considered to be promising applications in portable electronics. In this study, silicon/carbon nanofiber (Si@CNF) core–shell electrode has been prepared by the coaxial electrospinning method. The precursors of polyimide (PI) were for the first time used to form the core–shell structure of Si@CNF, which depicts outstanding flexibility and mechanical strength. The effect of doping concentrations of silicon (Si) nanoparticles embedded in the fiber is investigated as a binder-free anode for lithium-ion batteries. A 15 wt% doped composite electrode demonstrates superior performance, with an initial reversible capacity of 621 mA h g−1 at the current density of 100 mA g−1 and a high capacity retention up to 200 cycles. The excellent cycling performance is mainly due to the carbonized PI core–shell structure, which not only can compensate for the insulation property of Si but also has the ability to buffer the volume expansion during the repeated charge–discharge process.