Despite their high energy density and fast-charging capability, severe volume expansion during repeated lithiation and delithiation remains a major challenge for the commercialization of silicon (Si) anodes. Although polymer binders constitute only a small fraction of the electrode (5–10 wt%), they play a critical role in enhancing the electrochemical performance of Si anodes. In this work, .. The resulting polyols are blended with poly(acrylic acid) (PAA) to form water-processable binders for Si-based anodes. Compared to conventional PAA binders, Si/C anodes employing the blended binders exhibit significantly improved electrochemical performance, including higher specific capacity and enhanced cycling stability. This study demonstrates that CO₂-based polymer binders represent a promising and sustainable strategy for developing high-performance binders for Si-based anodes.