Ultrahigh-water-content biocompatible gelatin-based hydrogels: Toughened through micro-sized dissipative morphology as an effective strategy.

Fabrication of simultaneously robust and superabsorbent gelatin-based hydrogels for biomedical applications still remains a challenge due to lack of locally dissipative points in the presence of large water content. Here, we apply a synthesis strategy through which water absorbency and energy dissipative points are separated, and toughening mechanism is active closely at the crack tip. For this, gelatin-based microgels (GeMs) were synthesized in a way that concentrated supramolecular interactions were present to increase the energy necessary to propagate a macroscopic crack. The microgels were interlocked to each other via both temporary hydrophobic associations and permanent covalent crosslinks, in which the sacrificial binds sustained the toughness due to the mobility of the junction zones and particles sliding. However, chemical crosslinking points preserved the integrity and fast recoverability of the hydrogel. Hysteresis increased strongly with increasing supramolecular interactions within the network. The prepared hydrogels showed energy loss and swelling ratio up to 3440 J. m and 830%, respectively, which was not achievable with conventional network fabrication methods. The microgels were also assessed for their in vivo biocompatibility in a rat subcutaneous pocket assay. Results of hematoxylin and eosin (H&E) staining demonstrated regeneration of the tissue around the scaffolds without incorporation of growth factors. Also, vascularization within the scaffolds was observed after 4 weeks implantation. These results indicate that our strategy is a promising method to manipulate those valuable polymers, which lose their toughness and applicability with increasing their water content.