A ureido-pyrimidinone (UPy)-functionalized poly(acrylic acid) grafted with poly(ethylene glycol)(PEG), designated PAU-g-PEG, was developed as a high performance polymer binder for Si anodes in lithium-ion batteries. By introducing both a ureido-pyrimidinone (UPy) unit, which is capable of self-healing through dynamic hydrogen bonding within molecules as well as with Si, and an ion-conducting PEG onto the side chain of the poly(acrylic acid), this water-based self-healable and conductive polymer binder can effectively accommodate the volume changes of Si, while maintaining electronic integrity, in an electrode during repeated charge/discharge cycles. The Si@PAU-g-PEG electrode retained a high capacity of 1,450.2 mAh g⁻¹ and a Coulombic efficiency of 99.4% even after 350 cycles under a C-rate of 0.5 C. Under a high C-rate of 3 C, an outstanding capacity of 2,500 mAh g⁻¹ was also achieved, thus demonstrating its potential for improving the electrochemical performance of Si anodes.