Nanofiber-structured hydrogels with robust mechanical properties are promising candidates for the development of multifunctional materials in advanced fields. However, creating such materials that combine the virtues of high elongation, robust strength, and good elasticity remains an enormous challenge. Here, we demonstrate a nature-inspired methodology to fabricate dermis-mimicking network structured electrospun nanofibrous hydrogels with robust mechanical properties by combining the advantages of sustainable plant-based zein and elastic waterborne polyurethane (WPU). The reversible hydrogen bonding and strong covalent bonding between zein and WPU molecules are constructed in the double-network (DN) structured nanofibrous hydrogels (NFHs) with tunable stretchability and strength. The resulting NFHs exhibit the integrated characteristics of a stretch of 683%, a fracture strength of 6.5 MPa, a toughness of 20.7 MJ m, and complete recovery from large deformation. This nature-inspired structural design strategy may pave the way for designing mechanically robust nanofibrous hydrogels in structurally adaptive and scalable form.Copyright © 2020 Elsevier Inc. All rights reserved.