Abstract
Silicon is widely recognized as a next-generation anode owing to its exceptional theoretical capacity, yet its practical deployment in lithium-ion batteries is constrained by severe volume expansion, particle fracture, loss of electrical percolation, and solid electrolyte interphase layer instability. Polymer-based strategies have emerged as accessible solutions to engineer extensive volume changes and interfacial compatibility, while preserving pathways for charge transport. Viscoelastic polymer binders dissipate stress, catechol-inspired chemistries strengthen adhesion and tailor interphases, and conductive polymers can function simultaneously as binder, electronic additive, and artificial SEI. This review describes these approaches through a structure-process-performance perspective, emphasizing practically relevant metrics, such as initial capacity, initial Coulombic efficiency, and long-term cycling stability. We organize the main section into (i) dopamine-derived interfacial engineering, (ii) self-healing three-dimensional network binders, and (iii) conductive-polymer-based designs. In the last section, we articulate the functional requirements of polymers in silicon anodes, outline the ideal structural designs, and provide forward-looking avenues for future lithium-ion battery anode research.