The development of flexible conductive elastomers integrating renewable feedstock, splendid mechanical property, and excellent weather resistance is of major interest and challenge. Here, a novel strategy is reported to construct the liquid‐free cellulose‐derived ionic conductive elastomer that is successfully applied in the wearable sensor and triboelectric nanogenerators (TENG). In this strategy, the ionic conductive elastomer with physical and chemical dual‐crosslinking network is prepared via in situ polymerization of the polymerizable deep eutectic solvent. The construction of dual‐crosslinking network improves the mechanical strength and toughness more than 2 times, and the cellulose contributes to forming the dense hydrogen bond crosslinking network that can improve the recyclability, anti‐freezing, and solvent‐resistance performance. Benefiting from these features, the ionic conductive elastomer is successfully applied in the wearable sensors and TENG for monitoring human motion, and in harvesting mechanical energy to convert into stable electrical outputs to light the LEDs, charge the capacitor, and power the electronic watch. The ionic conductive elastomer maintains reliable sensing and energy harvesting performance even after recycling, soaking in organic solvent, or at low/high temperature. This study paves a promising strategy for fabricating sustainable and multifunction flexible electronics that are suitable for harsh environments.

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Sustainable shape-memory and self-healing elastomers with semi-interpenetrating network were prepared by a simple, efficient, and green bulk radical polymerization of ethyl cellulose, furfural, and fatty-acid-derived monomers. This approach could in situ one-pot form a semi-interpenetrating network elastomer with properties combining multiple-shape-memory and self-healing under solvent-free conditions. These elastomers were found to possess excellent multiple-shape-memory properties toward temperature, water, THF, and methanol. Moreover, the multiple-shape-memory properties could assist the self-healing of these elastomers, which was triggered by heating. Self-healing behavior studies showed that the presence of linear polymers in these elastomers could significantly improve the self-healing performance. This work provides a facile, efficient, and green approach in a solvent-free system to design new-generation sustainable, green, and functional materials.