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There is a growing interest in developing stretchable strain sensors to quantify the large mechanical deformation and strain associated with the activities for a wide range of species. Herein, we constructed elastomeric, healable hydrogen-bonded interpolymer complex (HIPC) rubberlike film by complexation of hydrogen-bond (H-bond)-donating poly(acrylic acid) (PAA) and H-bond-accepting poly(ethylene oxide) (PEO) (or poly(ethylene oxide)-poly(propylene oxide)-poly(ethylene oxide) (F108)). All HIPC elastomers prepared from varied PAA/PEO (or PAA/F108) ratios are healable elastomers with high extensibility (with the highest strain of 1400%). Recovery of all films can automatically occur or be accelerated by externally added water droplet. The stress- and strain healing efficiencies (η σ and η ε ) of the water-assisting healed PAA/F108 blends are as high as 99%. Furthermore, stretchable and healable conductor films were fabricated from silver nanowire-printed (Ag-p) and the single-walled carbon nanotube-blended (SW-b) conductor films, respectively. The healable Ag-p conductor film is an ultrasensitive strain sensor, exhibiting large electric resistance variation when stretched. In contrast, the healable SW-b film is an ultrastable strain sensor with reversible resistance strain response over 200 stretching release cycles within a high strain range of 500%. Therefore, this study provides a new and flexible HIPC strategy for the fabrication of stretchable, ultrasensitive, and stable self-healing electrode materials.

Highly Stretchable, Self-Healable Elastomers from Hydrogen-Bonded Interpolymer Complex (HIPC) and Their Use as Sensitive, Stable Electric Skin