Ultrahigh‐Water‐Content, Superelastic, and Shape‐Memory Nanofiber‐Assembled Hydrogels Exhibiting Pressure‐Responsive Conductivity

High-water-content hydrogels that are both mechanically robust and conductive could have wide applications in fields ranging from bioengineering and electronic devices to medicine; however, creating such materials has proven to be extremely challenging. This study presents a scalable methodology to prepare superelastic, cellular-structured nanofibrous hydrogels (NFHs) by combining alginate and flexible SiO2 nanofibers. This approach causes naturally abundant and sustainable alginate to assemble into 3D elastic bulk NFHs with tunable water content and desirable shapes on a large scale. The resultant NFHs exhibit the integrated properties of ultrahigh water content (99.8 wt%), complete recovery from 80% strain, zero Poisson's ratio, shape-memory behavior, injectability, and elastic-responsive conductivity, which can detect dynamic pressure in a wide range (>50 Pa) with robust sensitivity (0.24 kPa-1 ) and durability (100 cycles). The fabrication of such fascinating materials may provide new insights into the design and development of multifunctional hydrogels for various applications.