Aqueous spinning of robust, self-healable, and crack-resistant hydrogel microfibers enabled by hydrogen bond nanoconfinement

Abstract Robust damage-tolerant hydrogel fibers with high strength, crack resistance, and self-healing properties are indispensable for their long-term uses in soft machines and robots as load-bearing and actuating elements. However, current hydrogel fibers with inherent homogeneous structure are generally vulnerable to defects and cracks and thus local mechanical failure readily occurs across fiber normal. Here, inspired by spider spinning, we introduce a facile, energy-efficient aqueous pultrusion spinning process to continuously produce stiff yet extensible hydrogel microfibers at ambient conditions. The resulting microfibers are not only crack-insensitive but also rapidly heal the cracks in 30 s by moisture, owing to their structural nanoconfinement with hydrogen bond clusters embedded in an ionically complexed hygroscopic matrix. Moreover, the nanoconfined structure is highly energy-dissipating, moisture-sensitive but stable in water, leading to excellent damping and supercontraction properties. This work creates opportunities for the sustainable spinning of robust hydrogel-based fibrous materials towards diverse intelligent applications.