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Due to their safety and sustainability, polysaccharides such as cellulose and chitosan have great potential to be the matrix of gel polymer electrolytes (GPE) for lithium-based batteries. However, they easily form hydrogels due to the large numbers of hydrophilic hydroxyl or amino functional groups within their macromolecules. Therefore, a polysaccharide-based amphiphilic gel, or organogel, is urgently necessary to satisfy the anhydrous requirement of lithium ion batteries. In this study, a PEGylated chitosan was initially designed using a chemical grafting method to make an GPE for lithium ion batteries. The significantly improved affinity of PEGylated chitosan to organic liquid electrolyte makes chitosan as a GPE for lithium ion batteries possible. A reasonable ionic conductivity (1.12 × 10⁻³ S cm⁻¹) and high lithium ion transport number (0.816) at room temperature were obtained by replacing commercial battery separator with PEG-grafted chitosan gel film. The assembled Li/GPE/LiFePO₄ coin cell also displayed a high initial discharge capacity of 150.8 mA h g⁻¹. The PEGylated chitosan-based GPE exhibits great potential in the field of energy storage.