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Silicon is a promising active material for lithium-ion batteries (LIBs) with a high theoretical capacity (∼4000 mA h g–1). However, there is a critical issue that the fabrication of the Si anode needs complicated and high-cost processes to alleviate the poor cyclic performance, such as nanostructuring. Furthermore, the Si anode requires a high component ratio of conductive agents and binder in the electrode. Herein, we report the fabrication of submicron Si particles coated by a polyacrylonitrile (PAN) layer with a highly polar nitrile group via a facile one-step wet ball-milling process. During the milling of Si particles in PAN solutions, PAN adheres to the Si surface and forms a nanometer coating layer. The nitrile groups of PAN enhance the electrolyte wettability and increase the lithium-ion pathways on the Si surface. These result in a stable solid electrolyte interphase (SEI) layer and reduce the internal resistance of the electrodes. Si anodes with an optimal particle size and PAN layer (SM-Si@PAN) exhibit a superior performance even at ultra-fast current density (50 A g–1). In addition, a full-cell with an NCM712 cathode shows an excellent performance.