3D‐Printing of Ultratough and Healable Elastomers

Abstract Although 3D‐printing has offered a promising solution for the freeform fabrication of complex, arbitrary structures, developing elastomeric materials that simultaneously possess mechanical robustness and self‐healing functionality remains a significant challenge. To address this, a 3D‐printable elastomer is reported by the strategic incorporation of hierarchical hydrogen bonding (acylsemicarbazide and carbamate) into the photoactive resin, thereby overcoming the traditional trade‐off between mechanical strength and dynamic functionality. The resulting elastomer exhibits ultra‐toughness (158.5 MJ m −3 ), with tensile strength and breaking strain of 49.6 MPa and 1136%, respectively. In addition, the acylsemicarbazide moieties endow the 3D‐printed elastomers with unique dynamic characteristics, including self‐healing capabilities and shape reconfigurability, thus significantly enhancing the design flexibility and versatility of complex structures.