Dual-Conductive Hydrogels via Graphene Oxide-Cellulose Molecular Engineering for High-Performance Bioelectronics

Hydrogels are promising candidates for bioelectronics because of their hierarchical architectures and tunable functionalities. However, simultaneously achieving high conductivity and robust mechanical/physicochemical properties remains a critical challenge. Herein, we develop a dual ion-electron conductive hydrogel through the molecular engineering of cellulose chains with graphene oxide (GO) in a ZnCl2-coordinated network. The optimized hybrid hydrogel exhibits an exceptional conductivity of 25.51 S m–1 and ultralow interfacial impedance. Strong hydrogen bonding between cellulose and GO enhances the mechanical strength, achieving a compressive stress of 2.58 MPa. The hybrid hydrogel exhibited self-healing capability, antifreezing properties (down to −110.5 °C), and drying resistance. When assembled as a pressure sensor, the hydrogel demonstrates a high gauge factor of 25.13 for strain sensing and maintains good signal consistency after 100 cycles. This work provides a universal strategy for designing conductive hydrogels for next-generation wearable bioelectronics.