The emerging applications of hydrogels in devices and machines require hydrogels to maintain robustness under cyclic mechanical loads. Whereas hydrogels have been made tough to resist fracture under a single cycle of mechanical load, these toughened gels still suffer from fatigue fracture under multiple cycles of loads. The reported fatigue threshold for synthetic hydrogels is on the order of 1 to 100 J/m². We propose that designing anti-fatigue-fracture hydrogels requires making the fatigue crack encounter and fracture objects with energies per unit area much higher than that for fracturing a single layer of polymer chains. We demonstrate that the controlled introduction of crystallinity in hydrogels can substantially enhance their anti-fatigue-fracture properties. The fatigue threshold of polyvinyl alcohol (PVA) with a crystallinity of 18.9 weight % in the swollen state can exceed 1000 J/m².

This article proposes an approach of 3D printing structures consisting of stretchable hydrogels bonded with UV curable polymers.

The adhesion of soft connective tissues (tendons, ligaments, and cartilages) on bones in many animals can maintain high toughness (∽800 J m⁻²) over millions of cycles of mechanical loads. Such fatigue-resistant adhesion has not been achieved between synthetic hydrogels and engineering materials, but is highly desirable for diverse applications such as artificial cartilages and tendons, robust antifouling coatings, and hydrogel robots. Inspired by the nanostructured interfaces between tendons/ligaments/cartilages and bones, we report that bonding ordered nanocrystalline domains of synthetic hydrogels on engineering materials can give a fatigue-resistant adhesion with an interfacial fatigue threshold of 800 J m⁻², because the fatigue-crack propagation at the interface requires a higher energy to fracture the ordered nanostructures than amorphous polymer chains. Our method enables fatigue-resistant hydrogel coatings on diverse engineering materials with complex geometries. We further demonstrate that the fatigue-resistant hydrogel coatings exhibit low friction and low wear against natural cartilages.

Nature builds biological materials from limited ingredients, however, with unparalleled mechanical performances compared to artificial materials, by harnessing inherent structures across multi‐length‐scales. In contrast, synthetic material design overwhelmingly focuses on developing new compounds, and fails to reproduce the mechanical properties of natural counterparts, such as fatigue resistance. Here, a simple yet general strategy to engineer conventional hydrogels with a more than 100‐fold increase in fatigue thresholds is reported. This strategy is proven to be universally applicable to various species of hydrogel materials, including polysaccharides (i.e., alginate, cellulose), proteins (i.e., gelatin), synthetic polymers (i.e., poly(vinyl alcohol)s), as well as corresponding polymer composites. These fatigue‐resistant hydrogels exhibit a record‐high fatigue threshold over most synthetic soft materials, making them low‐cost, high‐performance, and durable alternatives to soft materials used in those circumstances including robotics, artificial muscles, etc.

Flexible and stretchable light emitting devices are driving innovation in myriad applications, such as wearable and functional electronics, displays and soft robotics. However, the development of flexible electroluminescent devices via conventional techniques remains laborious and cost-prohibitive. Here, we report a facile and easily-accessible route for fabricating a class of flexible electroluminescent devices and soft robotics via direct ink writing-based 3D printing. 3D printable ion conducting, electroluminescent and insulating dielectric inks were developed, enabling facile and on-demand creation of flexible and stretchable electroluminescent devices with good fidelity. Robust interfacial adhesion with the multilayer electroluminescent devices endowed the 3D printed devices with attractive electroluminescent performance. Integrated our 3D printed electroluminescent devices with a soft quadrupedal robot and sensing units, an artificial camouflage that can instantly self-adapt to the environment by displaying matching color was fabricated, laying an efficient framework for the next generation soft camouflages.