3D-Printed Multi-Stimulus-Responsive Hydrogels: Fabrication and Characterization

Stimulus-responsive hydrogels have broad applications in the biomedical, sensing, and actuation fields. However, conventional fabrication methods are often limited to 2D structures, hindering the creation of complex, personalized 3D hydrogel architectures. Furthermore, hydrogels responding to only a single stimulus and delays in fabrication techniques restrict their practical utility in biomedicine. In this study, we developed two novel multi-stimuli-responsive hydrogels (based on Gelatin/Sodium Alginate and Tannic Acid/EDTA-FeNa complexes) specifically designed for direct ink writing (DIW) 3D printing. We systematically characterized the printed properties and optimized component ratio, revealing sufficient mechanical strength (e.g., tensile modulus: Gel/SA-TA ≥ 0.22854 ± 0.021 MPa and Gel/SA-TA@Fe³⁺ ≥ 0.35881 ± 0.021 MPa), high water content (e.g., water absorption rate Gel/SA-TA ≥ 70.21% ± 1.5% and Gel/SA-TA@Fe³⁺ ≥ 64.86% ± 1.28%), excellent biocompatibility (e.g., cell viability: Gel/SA-TA and Gel/SA-TA@Fe³⁺ ≥ 90%) and good shape memory performance (e.g., the highest shape recovery rate of Gel/SA-TA reaches 74.85% ± 4.776%). Furthermore, we explored electrical characteristics, showing that the impedance value of Gel/SA-TA@Fe³⁺ hydrogel changes significantly under finger bending and NIR irradiation. This investigation demonstrates the potential of these 3D-printed multi-stimuli hydrogels for applications such as wearable flexible strain sensors.