This study focuses on the surface engineering of binder‐free anodes composed of Bi, Se, Cu, and carbon nanotubes to enhance Lithium‐ion batteries. The anodes synthesized in this study showed promising electrochemical properties. However, issues with cycle stability, operational speed, and solid electrolyte interface (SEI) formation affected their overall performance. To address these challenges, the study applied different conductive polymers, namely PEO, CMC, and PEGDA‐co‐VC, to form artificial SEI layers. The application of these polymers altered the stability and efficiency of the electrodes, with the PEGDA‐co‐VC‐coated electrodes demonstrating significant stability and consistent capacity over numerous cycles.