Low‐Temperature Extrusion of Waterborne Polyurethane–Polycaprolactone Composites for Multi‐Material Bioprinting of Engineered Elastic Cartilage

3D bioprinting of elastic cartilage tissues that are mechanically and structurally comparable to their native counterparts, while exhibiting favorable cellular behavior, is an unmet challenge. A practical solution for this problem is the multi-material bioprinting of thermoplastic polymers and cell-laden hydrogels using multiple nozzles. However, the processing of thermoplastic polymers requires high temperatures, which can damage hydrogel-encapsulated cells. In this study, the authors developed waterborne polyurethane (WPU)-polycaprolactone (PCL) composites to allow multi-material co-printing with cell-laden gelatin methacryloyl (GelMA) hydrogels. These composites can be extruded at low temperatures (50-60 °C) and high speeds, thereby reducing heat/shear damage to the printed hydrogel-capsulated cells. Furthermore, their hydrophilic nature improved the cell behavior in vitro. More importantly, the bioprinted structures exhibited good stiffness and viscoelasticity compared to native elastic cartilage. In summary, this study demonstrated low-temperature multi-material bioprinting of WPU-PCL-based constructs with good mechanical properties, degradation time-frames, and cell viability, showcasing their potential in elastic cartilage bio-fabrication and regeneration to serve broad biomedical applications in the future.