Fig. 1: Schematic aqueous pultrusion spinning of robust hydrogel microfibers with hydrogen bond nanoconfinement.

a Schematic spider spinning into high-performance silks with a hierarchical nanoconfinement structure that consists of highly conserved β-sheet nanocrystals as hard and strong domains as well as soft and ductile amorphous matrix. b Schematic continuous pultrusion spinning of PDMAEA-Q/PMAA hydrogel microfibers with spider silk-like nanoconfinement. With excess water evaporation at ambient conditions (25 °C, RH 60%), the gradual self-association of PMAA chains takes place generating high-density H-bond clusters embedded in the ionically complexed hygroscopic PDMAEA-Q/PMAA matrix. The calculated interaction energies (Einteraction) of H-bond cluster and ionic complexation from molecular dynamics simulation are also shown (Ha = Hartree). Note that, the ion pair between PDAMEA-Q and PMAA is water-separated; however, for clarity, water molecules are not displayed in this paper. c A rough comparison of the stiffness, elongation, moisture sensitivity, self-healability, fracture energy, damping capacity, and supercontraction properties of the present hydrogel microfiber with spider silk (data in Supplementary Table 1). Source data are provided as a Source Data file.