Conductive hydrogels (CHs) have been highlighted in the design of flexible strain sensors and stretchable triboelectric nanogenerators (TENGs) on the basis of their excellent physicochemical properties such as large stretchability and high conductivity. Nevertheless, the incident freezing and drying behaviors of CHs by using water solvent as the dispersion medium limit their application scopes significantly. Herein, an environment tolerant and ultrastretchable organohydrogel is demonstrated by a simple solvent‐replacement strategy, in which the partial water in the as‐synthesized polyacrylamide/montmorillonite/carbon nanotubes hydrogel is replaced with the glycerol, leading to excellent temperature toleration (−60 to 60 °C) and good stability (30 days under normal environment) without sacrificing the stretchability and conductivity. The organohydrogel exhibits an ultrawide strain sensing range (0–4196%) with a high sensitivity of 8.5, enabling effective detection and discrimination of human activities that are gentle or drastic under various conditions. Furthermore, the organohydrogel is assembled in a single‐electrode TENG, which displays excellent energy harvesting ability even under a stretchability of 500% and robustness to directly power wearable electronics in harsh cold conditions. This work inspires a simple route for multifunctional organohydrogel and promises the practical application of flexible and self‐powered wearable devices in extreme environments.

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Surface-enhanced Raman spectroscopy (SERS) technology has been regarded as a most efficient and sensitive strategy for the detection of pollutants at ultra-low concentrations. Fabrication of SERS substrates is of key importance in obtaining the homogeneous and sensitive SERS signals. Cellulose filter papers loaded with plasmonic metal NPs are well known as cost-effective and efficient paper-based SERS substrates. In this manuscript, face-to-face assembly of silver nanoplates via solvent-evaporation strategies on the cellulose filter papers has been developed for the SERS substrates. Furthermore, these developed paper-based SERS substrates are utilized for the ultra-sensitive detection of the rhodamine 6G dye and thiram pesticides. Our theoretical studies reveal the creation of high density hotspots, with a huge localized and enhanced electromagnetic field, near the corners of the assembled structures, which justifies the ultrasensitive SERS signal in the fabricated paper-based SERS platform. This work provides an excellent paper-based SERS substrate for practical applications, and one which can also be beneficial to human health and environmental safety.