The Mg-ion battery faces significant limitations due to its liquid electrolyte, which suffers from inherent issues such as leakage and the growth of Mg dendrites. In contrast, gel polymer electrolytes (GPEs) offer heightened safety, a wide voltage window, and excellent flexibility, making them a promising alternative with outstanding electrochemical performance. In this study, a cyano-modified cellulose (CEC) GPE was engineered to aim at enhancing ion transportation and promoting uniform ion-flux through interactions between N and Mg2+ ions. The resulting CEC-based GPE demonstrated a high ionic conductivity of 1.73 mS cm(-1) at room temperature. Furthermore, it exhibited remarkable Mg plating/stripping performance (coulombic efficiency similar to 96.7 %) and compatibility with electrodes. Importantly, when employed in a Mo6S8//Mg battery configuration, the CEC GPE displayed exceptional cycle stability, with virtually no degradation observed even after 650 cycles at 1C, thereby significantly advancing Mg-ion battery technology due to its excellent electrochemical properties. This study provides valuable insights into the molecular engineering of cellulose-based GPEs.
