Engineering Tough and Elastic Polyvinyl Alcohol‐Based Hydrogel with Antimicrobial Properties

Hydrogels have been extensively used for tissue engineering applications due to their versatility in structure and physical properties, which can mimic native tissues. Although significant progress has been made towards designing hydrogels for soft tissue repair, engineering hydrogels that resemble load-bearing tissues is still considered a great challenge due to their specific mechano-physical demands. Here, we report microporous, tough, yet highly compressible poly(vinyl alcohol) (PVA)-based hydrogels for potential applications in repairing or replacing different load-bearing tissues. The synergy of freeze-thawing and the Hofmeister effect, which controlled the spatial arrangement and aggregation of polymer chains, facilitated the formation of micro-structured frameworks with tunable porosity. While the maximum mechanical strength, toughness, and stretchability of the engineered hydrogel were ~390 kPa, ~388 kJ/m3, and ~170%, respectively, the Young's modulus based on compression testing was found to be in the range of ~0.02 - 0.30 MPa, highlighting the all-in-one mechanically enriched nature of the hydrogel system. Furthermore, the minimal swelling and degradation rate of the engineered hydrogel met the specific requirements of load-bearing tissues. Finally, excellent antibacterial resistance as well as in vitro biocompatibility of the hydrogel demonstrated its potential for the replacement of load-bearing tissues.