Polyaniline (PANi) hydrogels often exhibit highly mechanical and electrochemical properties, which have received extensive attention in the fields of batteries, supercapacitors, and sensors. However, the shortcomings such as hydrophobicity and easy aggregation of PANi frequently result in deterioration of mechanical and electrochemical performance of PANi hydrogels. Here, a bifunctional natural product, glycyrrhizic acid (GL), is utilized to prepare the homogeneous conductive PANi hydrogel, because GL not only can assemble into supramolecular hydrogel as the biocompatible matrix but also can salinize aniline monomers to facilitate the polymerization in situ to form uniformly dispersed PANi within GL matrix. Accordingly, the resulting GL/PANi hydrogel shows the Tyndall effect caused by the nanoclusters entangled by nanofibers and exhibits an improved storage modulus G′ (3.2 kPa) and loss modulus G″ (0.9 kPa), as well as the expected conductivity (0.17 S·m–1). In addition, the GL/PANi hydrogel is further reinforced by blending poly(vinyl alcohol) (PVA) for the required strength and stretchability as a flexible strain sensor. The results reveal that the obtained PVA/GL/PANi hydrogel has a fracture stress of 693 kPa at an elongation of 329%, with a fracture toughness of 82 MJ·m–3 and Young’s modulus of 47.9 kPa. Its gauge factor (GF) is measured to be 2.5 at lower strain (<130%) and up to 4.3 at larger strain (>130%). This good sensitivity and sensing stability make the PVA/GL/PANi hydrogel effectively monitor relevant human motion detections. Our work provides an innovative strategy to manufacture the homogeneous conductive PANi hydrogel for high-performance soft electronic devices.

Dynamic cross-linked biobased vitrimers can be recycled, reprocessed, and degraded via bond exchange reactions. However, the competitive raw materials and the tedious preparation process still bring challenges for these sustainable...