Robust zwitterionic hydrogels enabled by consolidated supramolecular networks and spatially hierarchical structures

Zwitterionic hydrogels have emerged as promising candidates for diverse applications, especially in epidermal electronics, due to their prominent hemocompatibility, superhydration, and nonfouling properties. However, their practical applications are often severely hindered by inadequate mechanical properties and limited functionalities. Here, we develop a mechanically robust zwitterionic hydrogel with an optimal combination of functions (RHOCF) by constructing a consolidated dynamic supramolecular framework and a spatially multiscale hierarchical structure. By finely introducing a reinforced entangled supramolecular network, along with hierarchical architectures across multiple length scales into the zwitterionic hydrogel system, we can engineer highly stiff and tough zwitterionic hydrogels that seamlessly integrate typically incompatible mechanical properties, including excellent stretchability, notable tensile strength, high fracture toughness, considerable stiffness, and great resilience. The RHOCF further integrates optical transparency, ionic conductivity, self-adhesion, and freezing tolerance, enabling conformal contact with dynamic, irregular surfaces for stable motion sensing and artifact-free electrophysiological signal acquisition. Zwitterionic hydrogels have potential in a range of applications due to favourable properties, but often mechanical properties are not suitable. Here, the authors report a hydrogel with an entangled supramolecular network for hierarchical networks, for zwitterionic materials with favourable material properties.