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Natural biopolymers feature natural abundance,diverse chemical compositions,tunable properties,easy processability,excellent biocompatibility and biodegradability,as well as nontoxicity,providing new opportunities for the development of flexible sensing and energy devices.Generally,biopolymers are utilized as the passive and active building blocks to endow the flexible devices with mechanical robustness and good biocompatibility.This review aims to provide a comprehensive review on natural biopolymer-based sensing and energy devices.The diverse structures and fabrication processes of three typical biopolymers,including silk,cellulose,and chitin/chitosan,are presented.We review their utilities as the supporting substrates/matrix,active middle layers,separators,electrolytes,and active components of flexible sensing devices (sensors,actuators,transistors) and energy devices (batteries,supercapacitors,triboelectric nanogenerators).Finally,the remaining challenges and future research opportunities are discussed.