A Strand Entangled Supramolecular PANI/PAA Hydrogel Enabled Ultra‐Stretchable Strain Sensor

Hydrogel electronics have attracted growing interest for emerging applications in personal healthcare management, human‐machine interaction, etc. Herein, a “doping then gelling” strategy to synthesize supramolecular PANI/PAA hydrogel with a specific strand entangled network is proposed, by doping the PANI with acrylic acid (AA) monomers to avoid PANI aggregation. The high‐density electrostatic interaction between PAA and PANI chains serves as a dynamic bond to initiate the strand entanglement, enabling PAA/PANI hydrogel with ultra‐stretchability (2830%), high breaking strength (120 kPa), and rapid self‐healing properties. Moreover, the PAA/PANI hydrogel‐based sensor with a high strain sensitivity (gauge factor = 12.63), a rapid responding time (222 ms), and a robust conductivity‐based sensing behavior under cyclic stretching is developed. A set of strain sensing applications to precisely monitor human movements is also demonstrated, indicating a promising application prospect as wearable devices. A strand entangled supramolecular polyacrylic acid/polyaniline (PAA/PANI) hydrogel is developed via a “doping then gelling” strategy. The designed high‐density electrostatic interaction between PAA and PANI chains endows the PAA/PANI hydrogel with ultra‐stretchability (2830%) and rapid self‐healing properties, thus achieving high strain sensitivity (GF = 12.63) for precisely monitoring human movements.