Improving the mechanical properties of 3D printed GelMA composite hydrogels by tannic acid

Abstract The lack of advanced biomaterials is a major challenge in bio‐printing. Gelatin‐methacryloyl (GelMA) hydrogel, as one of the most commonly used biomaterials in 3D printing, has limited the applications of medicine because of its low mechanical properties. In this study, to enhance the mechanical strength of GelMA hydrogels, we prepared a composite hydrogel based on F127 diacrylate (F127DA) and GelMA, followed by lyophilization and tannic acid (TA) treatment. In this composite hydrogel, the F127DA could self‐assemble into nanomicelles as crosslinking centers for monomer polymerization, which provides additional energy dissipation in hydrogels due to the synergistic deformation of micelles and internal rearrangement of physical binding. After lyophilization of the composite hydrogel, the porous hydrogel was formed. The subsequent treatment of TA could diffuse into the inner of the hydrogel and react with the hydrogel via hydrogen bonds, resulting in the significant enhancement of mechanical properties. The maximum tensile deformation of the obtained hydrogel was about 11 times higher than that of GelMA. This work demonstrates a method to enhance the mechanical properties of 3D‐printed GelMA hydrogel with promising application in bioprinting.