High-performance eco-friendly soft actuators showing large displacement, fast response, and long-term operational capability require further development for next-generation bioinspired soft robots. Herein, we report an electro-ionic soft actuator based on carboxylated cellulose nanocrystals (CCNC) and carboxylated cellulose nanofibers (CCNF), graphene nanoplatelets (GN), and ionic liquid (IL). The actuator exhibited exceptional actuation performances, achieving large displacements ranging from 1.6 to 12.3 mm under ultralow actuation voltages of 0.25–1.5 V. It also operated stably across a broad frequency band from 0.1 to 10 Hz and displayed a significant working stability of 99.3% after up to 240 cycles. Remarkably, the electro-active actuator demonstrated a fast response (0.39 s delay under 1.0 V at 0.1 Hz), and a long lifespan (with only a minor decrease of 2% for 2 years). The enhanced actuation performances of the actuator were attributed to its superior ionic conductivity, high charge storage ability, strong ionic interaction, and physical-chemical cross-linked networks. Furthermore, we successfully demonstrated the bioinspired applications of CCNC/CCNF-IL-GN actuators including micro-grippers, spiral-structure electroactive stents, biomimetic fingers, and bionic dragonfly wings. The proposed actuator and its bioinspired robot designs could offer a significant way for the development of next-generation eco-friendly soft actuators, soft robots, and biomedical microdevices in microenvironments requiring low-voltage environment.
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