Engineering Thermo-Responsive Hydrogels with Tailored Mechanics for Biomedical Integration

Poly(N-isopropylacrylamide) (PNIPAAm) hydrogels exhibit temperature-responsive volume changes near physiological temperature, but their low mechanical strength in the swollen state limits use in structurally demanding biomedical applications. In this study, we systematically investigated poly(NIPAAm-co-acrylamide), P(NIPAAm-co-AAm), hydrogels with varying AAm-to-NIPAAm ratios to explore the compositional trade-offs between thermal responsiveness and mechanical performance. Hydrogels were synthesized under fixed crosslinker and water content conditions, and evaluated through compressive mechanical testing, thermal swelling analysis, and crosslinking density estimation. Our results show that increasing AAm content enhances mechanical strength and stiffness but reduces the magnitude of temperature-induced volumetric shrinkage. An intermediate comonomer formulation demonstrated an optimal balance, maintaining both sufficient mechanical integrity for transdermal microneedle insertion and a reversible volume transition. This study highlights the potential of compositional tuning in hydrogel systems to meet the competing demands of responsiveness and durability in advanced biomedical applications.