Ultra-tough and super-robust hydrogel constructed through carbon dots induced crystallization domains integrated orientation regulation based on “pinning effect”

In this study, we present a novel strategy in which carbon dots (CDs) are employed to induce the formation of crystalline domains and further fabricated super-strong hydrogels with high crystallinity, distinct anisotropic structures and dense networks based on “pinning effect”, specifically, CDs act as nanofillers and heterogeneous nucleating agents. As-prepared hydrogels exhibited exceptional swelling resistance, ultra-high tensile strength (156 MPa) and toughness (225.2 MJ m ^− 3 ), surpassing most of other tough polymers, including natural tendons, plastic, synthetic rubber and artificial spider silk, etc. Notably, the hydrogel can support loads up to approximately 1.5×10 ⁵ times its own weight, highlighting their exceptional load-bearing capacity. Moreover, this strategy can be generalized to other CDs and adapted to environments with more stringent mechanical loads. This work not only offers new insights into the fabricating of ultra-robust hydrogels but also lays a foundation for the design and development of smart materials for underwater sensing.