Flexible and soft bioelectronics used on skin tissue have attracted attention for the monitoring of human health. In addition to typical metal-based rigid electronics, soft polymeric materials, particularly conductive hydrogels, have been actively developed to fabricate biocompatible electrical circuits with a mechanical modulus similar to biological tissues. Although such conductive hydrogels can be wearable or implantable in vivo without any tissue damage, there are still challenges to directly writing complex circuits on the skin due to its low tissue adhesion and heterogeneous mechanical properties. Herein, we report cellulose-based conductive hydrogel inks exhibiting strong tissue adhesion and injectability for further on-skin direct printing. The hydrogels consisting of carboxymethyl cellulose, tannic acid, and metal ions (e.g., HAuCl₄) were crosslinked via multiple hydrogen bonds between the cellulose backbone and tannic acid and metal-phenol coordinate network. Owing to this reversible non-covalent crosslinking, the hydrogels showed self-healing properties and reversible conductivity under cyclic strain from 0 to 400%, as well as printability on the skin tissue. In particular, the on-skin electronic circuit printed using the hydrogel ink maintained a continuous electrical flow under skin deformation, such as bending and twisting, and at high relative humidity of 90%. These printable and conductive hydrogels are promising for implementing structurally complicated bioelectronics and wearable textiles.

In bioelectronics, stretchable and self-healable electrodes can reliably measure electrophysiological signals from the human body because they have good modulus matching with tissue and high durability. In particular, the polymer–graphene composite has advantages when it is used as an electrode for bioelectronic sensor devices. However, it has previously been reported that external stimuli such as heat or light are required for the self-healing process of polymer/graphene composites. In this study, we optimized a conducting composite by mixing a self-healing polymer (SHP) and graphene. The composite materials can not only self-heal without external stimulation but also have rapid electrical recovery from repeated mechanical damage such as scratches. In addition, they had stable electrical endurance even when the cyclic test was performed over 200 cycles at 50% strain, so they can be useful for a bioelectronic sensor device with high durability. Finally, we measured the electromyogram signals caused by the movement of arm muscles using our composite, and the measured data were transmitted to a microcontroller to successfully control the movement of the robot’s hand.

Liquid metals not only have the electrical property of conductivity, but they also have a unique characteristic of existing in a liquid state at room temperature, unlike ordinary stiff solid metals. However, in bioelectronics, the modulus matching well between a device and skin or tissue is considered very advantageous, because high-quality biological signals can be recorded. Therefore, it is possible to implement soft electronics with stable and robust electrical characteristics by using LM as a conductive liquid-state filler. In this study, we changed a type of liquid metal, Eutectic Gallium Indium (EGaIn), into a particle form via tip sonication and mixed it with a solution that dissolved Styrene-Ethylene-Butylene-Styrene (SEBS) in toluene to fabricate a composite. The EGaIn-SEBS composite has high conductivity, excellent electrical durability under mechanically harsh conditions, and a degree of modulus similar to that of bare SEBS, which is lower than that of solid-filler-based SEBS composite. Finally, we demonstrated electrocardiogram signal monitoring using an EGaIn-Alginate two-layer electrode (EATE) that was fabricated by simply coating the surface of the composite with alginate hydrogel, which demonstrates excellent performance in bioelectronics.

In wearable bioelectronics, various studies have focused on enhancing prosthetic control accuracy by improving the quality of physiological signals. The fabrication of conductive composites through the addition of metal fillers is one way to achieve stretchability, conductivity, and biocompatibility. However, it is difficult to measure stable biological signals using these soft electronics during physical activities because of the slipping issues of the devices, which results in the inaccurate placement of the device at the target part of the body. To address these limitations, it is necessary to reduce the stiffness of the conductive materials and enhance the adhesion between the device and the skin. In this study, we measured the electromyography (EMG) signals by applying a three-layered hydrogel structure composed of chitosan–alginate–chitosan (CAC) to a stretchable electrode fabricated using a composite of styrene–ethylene–butylene–styrene and eutectic gallium-indium. We observed stable adhesion of the CAC hydrogel to the skin, which aided in keeping the electrode attached to the skin during the subject movement. Finally, we fabricated a multichannel array of CAC-coated composite electrodes (CACCE) to demonstrate the accurate classification of the EMG signals based on hand movements and channel placement, which was followed by the movement of the robot arm.

Soft bioelectronic systems with a unique mechanical property, namely modulus matching between human skin (or tissue) and the device, have gained widespread attention. This is because of their closed-loop strain-insensitive electrical performance ranging from application in the long-term stable measurements of physiological signals and feedback modulation to human skin (or organs). Various materials and integration/fabrication strategies such as buckled, rigid islands, and wavy designs addressed for soft bioelectronic systems require complex device fabrication with time-consuming packaging and integration processes. In this study, we developed a soft bio-integrated multifunctional device (SBMD) fabricated through the simple thermal evaporation and transfer processes. The intrinsically stretchable Au–SEBS film composed of thermally evaporated gold (Au) nanomembranes and an elastomeric substrate was applied to various functional modules that are capable of sensing the strain (up to ~300%), temperature (with a thermal sensitivity of ~0.6 Ω/°C), chemicals (at a concentration of NaCl of ~0.5 wt%), and even electrophysiological cardiac/muscle signals and showing thermal actuations (80 °C at 9 V). Specifically, such multifunctions of the SBMD were stably performed even on skin. Thus, we believe the SBMD would be a promising candidate for realizing soft bioelectronic systems.