Biomimetic Elastomer–ClayNanocomposite Hydrogelswith Control of Biological Chemicals for Soft Tissue Engineering andWound Healing

Resilient hydrogels are of great interest in soft tissue applications, such as soft tissue engineering and wound healing, with their biomimetic mechanical and hydration properties. A critical aspect in designing hydrogels for healthcare is their functionalities to control the surrounding biological environments to optimize the healing process. Herein, we have created an elastomer–clay nanocomposite hydrogel system with biomimetic mechanical behavior and sustained drug delivery of bioactive components and malodorous diamine-controlling properties. These hydrogels were prepared by a combined approach of melt intercalation of poly­(ethylene glycol) and montmorillonite clay, followed by <i>in situ</i> cross-linking with a branched poly­(glycerol sebacate) prepolymer. The hydration, vapor transmission, and surface wettability of the hydrogels were readily controlled by varying the clay content. Their mechanical properties were also modulated to mimic the Young’s moduli (ranging between 12.6 and 105.2 kPa), as well as good flexibility and stretchability of soft tissues. A porous scaffold with interconnected pore structures as well as full and instant shape recovery was fabricated from a selected nanocomposite to demonstrate its potential applications as soft tissue scaffolds and wound healing materials. Biodegradability and biocompatibility were tested <i>in vitro</i>, showing controllable degradation kinetics with clay and no evidence of cytotoxicity. With the high surface area and absorption capacity of the clay, sustained drug delivery of a proangiogenic agent of 17β-estradiol as a model drug and the ability to control the malodorous diamines were both achieved. This elastomer–clay nanocomposite hydrogel system with a three-dimensional interconnected porous scaffold architecture and controllable hydration, mechanical, and biodegradable properties, as well as good biocompatibility and the ability to control the biological chemical species of the surrounding environments, has great potential in soft tissue engineering and wound healing.