Muscle‐Inspired Robust Anisotropic Cellulose Conductive Hydrogel for Multidirectional Strain Sensors and Implantable Bioelectronics

Abstract Integrating superior mechanical performance, anisotropic conductivity, and biocompatibility into conductive hydrogels as all‐in‐one human‐machine interaction device remains challenging. Herein, by mimicking the anisotropic structures of human muscles, a robust anisotropic conductive hydrogel is developed by initially aligning polyvinyl alcohol with polypyrrole decorated cellulose nanofibrils to form an anisotropically oriented polymer networks, followed by post‐crosslinking with tannic acid (TA). Introducing TA into hydrogel network permanently secures its hierarchically anisotropic structure through multiple hydrogen bonds, thus endowing the hydrogel with exceptional mechanical properties (tensile strength of 11.41 MPa, toughness of 12.44 MJ m − 3 ), anisotropic adhesive property, and direction‐dependent conductivity. With these attributes, a hydrogel strain sensor with excellent multidirectional sensitivity is developed, enabling stable monitoring of multi‐degrees of freedom joint movements in the human body and facilitating the control of a multiaxial virtual robot manipulator. Moreover, the in vitro/vivo tests demonstrate exceptional biocompatibility and anti‐biofouling properties of the as‐prepared hydrogel sensor, maintaining stable electronic response signals for over 14 days after successful implantation into the Achilles tendon of mice. Overall, this study presents a promising approach for designing conductive hydrogels with superior mechanical properties and anisotropic functionality for emerging applications in both in vitro and in vivo human‐machine interface materials.