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Growing concern regarding the impact of fossil fuels has led to demands for the development of green and renewable materials for advanced electrochemical energy storage devices. Biopolymers with unique hierarchical structures and physicochemical properties, serving as an appealing platform for the advancement of sustainable energy, have found widespread application in the gel electrolytes of supercapacitors. In this Review, we outline the structure and characteristics of various biopolymers, discuss the proposed mechanisms and assess the evaluation metrics of gel electrolytes in supercapacitor devices, and further analyze the roles of biopolymer materials in this context. The state-of-the-art electrochemical performance of biopolymer-based hydrogel electrolytes for supercapacitors and their multiple functionalities are summarized, while underscoring the current technical challenges and potential solutions. This Review is intended to offer a thorough overview of recent developments in biopolymer-based hydrogel electrolytes, highlighting research concerning green and sustainable energy storage devices and potential avenues for further development., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)