Ultrathin and ultrastrong hydrogel bioelectronic membranes

Hydrogels are promising materials for constructing next-generation bioelectronics because of their excellent biocompatibility and mechanical compliance. Yet, creating robust and multifunctional hydrogel devices that conform to the surface of 3D organs remains challenging. Here, we report a biomimetic strategy for engineering ultrathin and ultrastrong hydrogel membranes as an advanced platform for organ-conformal bioelectronics. In these hydrogels, self-organized nanofiber networks confer strain-stiffening characteristics with a phenomenal combination of high mechanical strength (∼13.65 MPa), fracture toughness (∼21 573 J/m²), and low initial stiffness (∼600 kPa), which accommodates the construction of ultrathin membranes (∼10 μm thickness) reconciling mechanical robustness and 3D conformability. Theoretical simulations reveal unique strengthening mechanisms originating from the topological reconfiguration of fibrillar joints, indicating a widely applicable principle for designing soft composites involving 3D fibrillar networks. We show that various electronic components, including conducting polymers and wafer-fabricated microelectronic sensors, can be integrated on the ultrathin hydrogel membranes, providing means for multimodal physiological sensing and stimulation. These hydrogel membranes open paths to robust, functional and biocompatible interfaces with 3D soft organs and tissues, which are useful for epidermal electronics, implantable brain-machine interfaces, peripheral nerve stimulation, and many other bioelectronic applications.