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.

Extrusion-based 3D-bioprinting using hydrogels has exhibited potential in precision medicine; however, researchers are beset with several challenges. A major challenge of this technique is the production of constructs with sufficient height and fidelity to support cellular behavior in vivo. In this study, we present the 3D-bioprinting of cylindrical constructs with tunable gelation kinetics by controlling the covalent crosslinking density and gelation time of a tyramine-functionalized alginate hydrogel (ALG-TYR) via enzymatic reaction by horseradish peroxidase (HRP) and hydrogen peroxide (H₂O₂). The extruded filament was crosslinked for a second time on a support bath containing H₂O₂ to increase fidelity after printing. The resulting tubular construct, with a height of 6 mm and a wall thickness of 2 mm, retained its mechanical properties and had a maximum 2-fold swelling after 2 d. Furthermore, collagen (COL) was introduced into the ALG-TYR hydrogel network to increase the mechanical modulus and cell cytocompatibility, as the encapsulated fibroblast cells exhibited a higher cell viability in the ALG-TYR/COL construct (92.13 ± 0.70%) than in ALG-TYR alone (68.18 ± 3.73%). In summary, a vascular ECM-mimicking scaffold was 3D-bioprinted with the ALG-TYR/COL hybrid hydrogel, and this scaffold can support tissue growth for clinical translation in regenerative and personalized medicine.

For recently devised wound-healing materials, a variety of acute application systems with sustainable therapeutic effects on wound sites have been suggested. For example, hydrogel-type healing agents with porous structures and high drug encapsulation efficiencies have been developed for wound repair. However, challenges remain about the poor mechanical and adhesive properties of hydrogels. Herein, we propose a punicalagin (PC)-containing wound-healing hydrogel in adhesive form that is mechanically stable and has sustainable wound-healing therapeutic efficiency. The APC hydrogel, composed of alginate (ALG), PC, and chitosan–gallol (CHI–G), exhibits significant mechanical and self-healing properties, thus indicating that PC increases cross-linking in ALG/CHI–G as macromolecule. The PC-containing mechanically enhanced hydrogel demonstrates high tissue adhesiveness. Sustainable PC release for 192 h, which indicates high therapeutic effect of the released PC, and great blood compatibility are evaluated based on rapid blood coagulation and minimal hemolysis. The cytocompatibility and wound-healing abilities of the PC-containing APC hydrogel are greater than those of the non-PC hydrogel, as verified by cell compatibility and wound scratch assays. These results indicate that a suitable concentration of PC-containing hydrogel with sustainable moisture condition and PC release may inspire further polyphenol-agent-containing hydrogels as wound-healing agents with structural stability and therapeutic efficiency.