Skin-like Heterogeneous and Self-Healing Conductive Hydrogel toward Ultrasensitive Marine Sensing

Flexible wearable electronic devices based on hydrophobic, conductive hydrogels have attracted widespread attention in the field of underwater sensing. However, traditional homogeneous hydrogels tend to compromise their conductivity and sensing performance when achieving hydrophobicity, and the high complexity of marine environments further reduces their sensing performance and service life. Here, we develop a seawater-resistant conductive hydrogel with ultrahigh sensitivity and self-healing ability by the introduction of a skin-like heterogeneous structure, consisting of a hydrophobic outer layer that protects against seawater and a conductive internal layer that senses. Based on a heterogeneous structure obtained through surface hydrophobic modification of confined nitrogen-alkylation reaction, the conductive hydrogel simultaneously achieves satisfying seawater resistance (contact angle of 123.2°), high ionic conductivity (2.86 S m–1), and excellent sensing sensitivity in seawater (GF = 6.15), harmonizing the contradiction between water resistance and sensing of traditional hydrophobic hydrogels. In addition, abundant hydrogen-bonding and dipole–dipole interactions endow the heterogeneous hydrogel with an outstanding self-healing ability, exhibiting high-efficiency self-healing behavior in seawater. Underwater strain sensors constructed with the heterogeneous hydrogel can be used for detecting human motion in simulated seawater environments and real-time signal transmission, showcasing their great potential as wearable electronic devices in the marine sensing field.