Bioinspired Ultratough Hydrogel with Fast Recovery, Self‐Healing, Injectability and Cytocompatibility

Inspired by the mussel byssus adhesiveness, a highly hydrated polymeric structure is designed to combine, for the first time, a set of interesting features for load‐bearing purposes. These characteristics include: i) a compressive strength and stiffness in the MPa range, ii) toughness and the ability to recover it upon successive cyclic loading, iii) the ability to quickly self‐heal upon rupture, iv) the possibility of administration through minimally invasive techniques, such as by injection, v) the swelling ratio being adjusted to space‐filling applications, and vi) cytocompatibility. Owing to these characteristics and the mild conditions employed, the encapsulation of very unstable and sensitive cargoes is possible, highlighting their potential to researchers in the biomedical field for the repair of load‐bearing soft tissues, or to be used as an encapsulation platform for a variety of biological applications such as disease models for drug screening and therapies in a more realistic mechanical environment. Moreover, given the simplicity of this methodology and the enhanced mechanical performance, this strategy can be expanded to applications in other fields, such as agriculture and electronics. As such, it is anticipated that the proposed strategy will constitute a new, versatile, and cost‐effective tool to produce engineered polymeric structures for both science and technology. Inspired by the mussel byssus attachment system, a self‐healable, ultratough and strong hydrogel is reported. The mild conditions employed during the fabrication process, as well as the use of nature‐based materials, make it a prospective candidate for a wide range of applications including in the biomedical field.