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Low‐cost and scalable processes to fabricate Si‐based anodes with high areal capacity and excellent cycling performance remain a challenge, thereby limiting their widespread application. Herein, we report Si nanoparticles@conductive carbon framework@polymer (Si@C@P) composite electrodes, in which Si nanoparticles are homogeneously immobilized within a three‐dimensional network of conductive carbon nanofibers bound by a high‐viscosity polymer. When used as anodes for lithium‐ion batteries, the obtained Si@C@P composite electrodes deliver an initial coulombic efficiency of 83.5 % and an areal capacity of 2.0 mAh cm−2 (1152 mAh gnormalenormallnormalenormalcnormaltnormalrnormalonormaldnormale-1 ), with a capacity retention about 0.8 mAh cm−2 (466 mAh gnormalenormallnormalenormalcnormaltnormalrnormalonormaldnormale-1 ) after 150 discharge–charge cycles at 0.1 C. This work provides a low‐cost route for the large‐scale manufacture of Si‐based anodes with high areal capacity, which may be very significant for the development of lithium‐ion batteries with high energy density.

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