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Flexible devices serve as important intelligent interfaces in various applications involving health monitoring, biomedical therapies, and human–machine interfacing. To address the concern of electronic waste caused by the increasing usage of electronic devices based on synthetic polymers, bio‐origin materials that possess environmental benignity as well as sustainability offer new opportunities for constructing flexible electronic devices with higher safety and environmental adaptivity. Herein, the bio‐source and unique molecular structures of various types of natural bio‐origin materials are briefly introduced. Their properties and processing technologies are systematically summarized. Then, the recent progress of these materials for constructing emerging intelligent flexible electronic devices including energy harvesters, energy storage devices, and sensors are introduced. Furthermore, the applications of these flexible electronic devices including biomedical implants, artificial e‐skin, and environmental monitoring are summarized. Finally, future challenges and prospects for developing high‐performance bio‐origin material‐based flexible devices are discussed. This review aims to provide a comprehensive and systematic summary of the latest advances in the natural bio‐origin material‐based flexible devices, which is expected to offer inspirations for exploitation of green flexible electronics, bridging the gap in future human–machine–environment interactions. [ABSTRACT FROM AUTHOR]

Abstract Flexible devices serve as important intelligent interfaces in various applications involving health monitoring, biomedical therapies, and human–machine interfacing. To address the concern of electronic waste caused by the increasing usage of electronic devices based on synthetic polymers, bio‐origin materials that possess environmental benignity as well as sustainability offer new opportunities for constructing flexible electronic devices with higher safety and environmental adaptivity. Herein, the bio‐source and unique molecular structures of various types of natural bio‐origin materials are briefly introduced. Their properties and processing technologies are systematically summarized. Then, the recent progress of these materials for constructing emerging intelligent flexible electronic devices including energy harvesters, energy storage devices, and sensors are introduced. Furthermore, the applications of these flexible electronic devices including biomedical implants, artificial e‐skin, and environmental monitoring are summarized. Finally, future challenges and prospects for developing high‐performance bio‐origin material‐based flexible devices are discussed. This review aims to provide a comprehensive and systematic summary of the latest advances in the natural bio‐origin material‐based flexible devices, which is expected to offer inspirations for exploitation of green flexible electronics, bridging the gap in future human–machine–environment interactions.