SGs‐CNTs/PAM/CCS Triple Network Hydrogel: Neural Architecture Inspired for Broadband EMI Shielding and Environmental Resilience

Abstract Improving traditional multi‐network hydrogels by introducing a low‐density rigid filler network to optimize a single ionic conductivity and overcome the limited electromagnetic properties to produce electromagnetic interference (EMI) shielding hydrogels is a pioneering challenge. Drawing inspiration from the neural network, this research introduces a novel triple‐network (TN) hydrogel. The single‐layer graphenes (SGs) and carbon nanotubes (CNTs) mimic the conductive channels similar to neurons and axons/dendrites, respectively, and assist the dispersion‐lap‐fixation process of the filler by carboxymethyl chitosan (CCS) and polyacrylamide (PAM). This collaborative assembly of SGs‐CNTs, coupled with the presence of water molecules, imparts SGs‐CNTs/CCS/PAM (SCCP) hydrogel with exceptional EMI shielding effectiveness (SE) across the 8.2–26.5 GHz range (X, Ku, and K bands), reaching SE of 42.31, 50.20, and 60.78 dB, respectively. Moreover, the photothermal properties of SGs‐CNTs enable CCS/PAM to heal sections efficiently and recover electromagnetic properties when exposed to near‐infrared (NIR) light. SCCP also boasts a significant depression of the freezing point to −43 °C, achieved through the hydration of LiCl. Boasting diversified manufacturing, self‐healing properties, and exceptional environmental durability, SCCP stands out as an ideal candidate for EMI shielding and shows excellent potential for multifunctional applications in flexible electronics.