Nitrogen‐Rich Azolate Framework‐Derived Porous Carbon Nanocomposite Hydrogels Shielding Material with Tunable Dynamic Bonding‐Induced Self‐Healing Properties

Abstract Conductive hydrogels are promising candidates for electromagnetic interference (EMI) shielding in flexible and wearable electronics, yet their practical implementation remains hindered by low‐temperature freezing and mechanical fragility. Although organohydrogels can enhance anti‐freezing performance, their compromised conductivity often reduces shielding efficiency. Here, a multifunctional Fe@C/TPS nanocomposite hydrogel engineered through the incorporation of nitrogen‐rich azolate framework–derived porous carbon is reported. The introduction of these nanomaterials simultaneously enhances ionic conductivity and mechanical robustness through strong interfacial interactions. As a result, the hydrogel achieves an outstanding EMI shielding effectiveness of 56.97 dB in the X‐band, alongside rapid strain response (response time: 200 ms, GF = 4.7). Remarkably, stable shielding and sensing performance are maintained even under harsh conditions, including −20 °C and 60% tensile strain, owing to the binary water–ethylene glycol solvent system that sustains a robust conductive network. Moreover, the dynamic hydrogen‐bonding interactions impart excellent self‐healing behavior, enabling over 92% recovery of the original shielding efficiency after mechanical damage.