Supramolecularly reinforced conductive dynamic disulfide elastomers for dual‐environment wearable sensing

Dynamic covalent adaptable networks, particularly thioctic acid (TA)‐derived systems, are renowned for their dynamicity and stimulus responsiveness, for example, self‐healing, yet their broader applications remain restricted by poor electrical conductivity and intrinsic hydrophobicity. Herein, we propose a unique strategy for fabricating supramolecularly crosslinked poly(disulfides), wherein polyethyleneimine facilitates the homogeneous aqueous dispersion of TA‐derived monomers and MXene nanosheets through cooperative supramolecular interactions, followed by evaporation‐induced polymerization to yield a highly crosslinked conductive elastomeric network. Owing to the uniformly distributed supramolecular crosslinking, the conductive elastomer exhibits MXene‐dependent reinforcement, achieving balanced strength and stretchability, alongside broad‐spectrum solvent resistance, robust and versatile adhesion, excellent biocompatibility and ambient self‐healing with quantitative mechanical recovery. The demonstrated piezoresistive sensing capability in both air and underwater environments underscores the promise of these conductive poly(disulfides) as advanced multifunctional sensing materials.