High‐performance electoactive artificial muscles with biofriendly, biodegradable, and biocompatible functionalities have attracted enormous attention in the era of human friendly electronic devices such as wearable electronics, soft haptic devices, and implantable or disposal biomedical devices. Here, a high‐fidelity bioelectronic soft actuator is reported based on biofriendly 2,2,6,6‐tetramethylpiperidine‐1‐oxyl radical‐oxidized bacterial cellulose (TOBC), chemically modified graphene, and ionic liquid [EMIM][BF4] as plasticizer, thereby realizing large deformable, faster, biodegradable, air working, and highly durable TOBC‐IL‐G muscular actuator. Especially, the TOBC‐IL‐G(0.10 wt%) membrane shows a dramatic increment of the ionic conductivity up to 120%, of specific capacitance up to 95%, of tensile modulus up to 63%, and of tensile strength up to 60%, for TOBC‐IL, resulting in 2.3 times larger bending deformation without serious back‐relaxation phenomena. The developed high‐performance and durable bioelectronic muscular actuator can be a promising candidate for satisfying the tight requirements of human‐related bioengineering as well as biomimetic robotics and biomedical active devices.

We report a high-performance electro-active hybrid actuator based on freeze-dried bacterial cellulose and conducting polymer electrodes. The freeze-dried bacterial cellulose, which has a sponge form, can absorb a much greater amount of ionic liquid, which is a prerequisite for dry-type and high-performance electro-active polymers. In addition, the poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT:PSS) conducting layers are deposited on the top and bottom surfaces of the freeze-dried bacterial cellulose using a simple dipping and drying method. The results show that the freeze-dried bacterial cellulose actuator with conducting polymer electrodes has a much larger tip displacement under electrical stimuli than pure bacterial cellulose actuators with metallic electrodes. The large bending displacement of the freeze-dried bacterial cellulose actuator under low input voltage is due to the synergistic effects of the ion migration of the dissociated ionic liquids inside the bacterial cellulose and the electrochemical doping processes of the PEDOT:PSS electrode layers.

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A novel electroactive biopolymer actuator was developed based on a cross-linked ionic networking membrane of TEMPO-oxidized bacterial cellulose nanofibers (TOCNs) and polyvinyl alcohol (PVA). Ionic liquids were added to develop an air-working artificial muscle and to enhance the performance of the PVA-TOCN actuator. Poly(3,4-ethylenedioxythiophene)poly(styrenesulfonate) (PEDOT:PSS) conducting layers were deposited on the top and bottom surfaces of the PVA-TOCN membrane via a simple dipping and drying method. The electroactive PVA-TOCN actuator under both step and harmonic electrical inputs shows much larger tip displacements and faster bending deformation than the pure TOCN actuator. The crosslinking reaction between PVA and TOCN was observed in the Fourier transform-near-infrared (FT-IR) spectrum of the PVA-TOCN networking membrane. Scanning electron microscopy (SEM), x-ray diffusion (XRD), thermogravimetric analysis (TGA) and tensile and ion conductivity testing results for the PVA-TOCN membrane were compared with those of pristine TOCN. Most important, the PVA-TOCN actuator shows much larger bending deformation under even extremely low input voltages, and this could be attributed to the cross-linking mechanism and the greater flexibility resulting from the synergistic effects between PVA and TOCN.