Living systems can respond to external stimuli by dynamic interface changes. Moreover, natural wrinkle structures allow the surface to switch dynamically and reversibly from flat to rough in response to specific stimuli. Artificial wrinkle structures have been developed for applications such as optical devices, mechanical sensors, and microfluidic devices. However, chemical molecule‐triggered flexible sensors based on dynamic surface wrinkling have not been demonstrated. Inspired by human skin wrinkling, herein, a volatile organic compound (VOC)‐responsive flexible sensor with a switchable dual‐signal response (transparency and resistance) is achieved based on a multilayered Ag nanowire (AgNW)/SiOx/polydimethylsiloxane (PDMS) film. Wrinkle structures can form dynamically in response to VOC vapors (such as ethanol, toluene, acetone, formaldehyde, and methanol) due to the instability of the multilayer induced by their different swelling capabilities. By controlling the modulus of PDMS and the thickness of the SiOx layer, tunable sensitivities in resistance and transparency of the device are achieved. Additionally, the proximity mechanism of the solubility parameter is proposed, which explains the high selectivity of the device toward ethanol vapor compared with that of other VOCs well. This stimuli‐responsive sensor exhibits the dynamic visual feedback and the quantitative electrical signal, which provide a novel approach for developing smart flexible electronics.

Flexible and stretchable electronics are emerging in mainstream technologies and represent promising directions for future lifestyles. Multifunctional stretchable materials with a self-healing ability to resist mechanical damage are highly desirable but remain challenging to create. Here, we report a stretchable macromolecular elastomeric gel with the unique abilities of not only self-healing but also transient properties at room temperature. By inserting small molecule glycerol into hydroxyethylcellulose (HEC), forming a glycerol/hydroxyethylcellulose (GHEC) macromolecular elastomeric gel, dynamic hydrogen bonds occur between the HEC chain and the guest small glycerol molecules, which endows the GHEC with an excellent stretchability (304%) and a self-healing ability under ambient conditions. Additionally, the GHEC elastomeric gel is completely water-soluble, and its degradation rate can be tuned by adjusting the HEC molecular weight and the ratio of the HEC to glycerol. We demonstrate several flexible and stretchable electronics devices, such as self-healing conductors, transient transistors, and electronic skins for robots based on the GHEC elastomeric gel to illustrate its multiple functions.