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The energy density of lithium-ion batteries (LIBs) can be meaningfully increased by utilizing Si-on-graphite composites (Si@Gr) as anode materials, because of several advantages, including higher specific capacity and low cost. However, long cycling stability is a key challenge for commercializing these composites. In this study, to solve this issue, we have developed a multifunctional polymeric artificial solid-electrolyte interphase (A-SEI) protective layer on carbon-coated Si@Gr anode particles (making Si@Gr/C-SCS) to prolong the cycling stability in LIBs. The coating is made of sulfonated chitosan (SCS) that is crosslinked with glutaraldehyde promoting good ionic conduction together with sufficient mechanical strength of the A-SEI. The focused ion beam-scanning electron microscopy and high-resolution transmission electron microscopy images show that the SCS is uniformly coated on the composite particles with thickness in nanometer. The anodes are investigated in Li metal cells Si@Gr/C-SCS||Li metal) and lithium-ion full-cells (LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM-622)||Si@Gr/C-SCS) to understand the material/electrode intrinsic degradation as well as the impact of the polymer coating on active lithium losses because of the continuous SEI (re)formation. The anode composites exhibit a high capacity reaching over 600 mAh g -1 , and even without electrolyte optimization, the Si@Gr/C-SCS illustrates a superior long cycle life performance of up to 1000 cycles (over 67% capacity retention). The excellent long-term cycling stability of the anodes was attributed to the SCS polymer coating acting as the A-SEI. The simple polymer coating process is highly interesting in guiding the preparation of long-cycle-life electrode materials of high-energy LIB cells.