Abstract
Through molecular design, this study developed a conformal self-healing organogel (CSHO) via molecular design. Utilizing acryloylmorpholine (ACMO) and hydroxyethyl acrylamide (HEAA) as monomers, tributyl citrate (TBC) as the solvent, and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) as an electrolyte salt, the organogel was polymerized by UV curing. A dual supramolecular network of hydrogen and lithium bonds provided excellent mechanical strength without chemical crosslinkers, while also enabling self-healing. TBC enhanced flexibility and established continuous ion channels, boosting ionic conductivity. The CSHO exhibited excellent conformability to complex surfaces, replicating fine textures, and was recyclable through a water-based process. Mechanical sensing tests showed that the CSHO could respond sensitively and in real time to pressing and stretching. This work presents a strategy for multifunctional ionic conductors, advancing flexible sensors and wearable devices.