Bioinspired flexible, high-strength, and versatile hydrogel with the fiberboard-and-mortar hierarchically ordered structure

The synthetic hydrogels with high water contents are promising for various applications, however, they usually exhibit low mechanical properties. In this work, inspired by the natural biological soft tissues, whose hierarchically ordered fibrous structures result in high strength and good flexibility, a flexible, high-strength, and versatile hydrogel with the fiberboard-and-mortar hierarchically ordered structure (HFMOS) is developed based on ultralong hydroxyapatite (HAP) nanowires and polyacrylic acid (PAA). The as-prepared HFMOS hydrogel has a high water content (~ 70 wt.%), dense structure, and excellent mechanical properties, and these properties are similar to those of the human cartilage and are superior to many hydrogels reported in the literature. The excellent mechanical properties of the HFMOS hydrogel originate from the combination of the fiberboard-and-mortar hierarchically ordered structure, reinforcement of ultralong HAP nanowires, strong interfacial strength, and multiple energy dissipation pathways. Moreover, thanks to the controllable components and injection procedure, the HFMOS hydrogel with a Janus structure is prepared for particular applications. The HFMOS hydrogel possesses abundant ordered water channels, and can be used for loading, release, and directed delivery of various functional substances. Thus, the as-prepared flexible, high-strength, and versatile HFMOS hydrogel possesses a great potential for various applications such as water purification, pollution treatment, biomedicine, nanofluidic devices, and high-performance structural materials.