Hydrogel electrolytes have attracted enormous attention in flexible and safe supercapacitors. However, the interfacial contact problem between hydrogel electrolyte and electrodes, and the environmental instability are the key factors restricting the development of hydrogel‐based supercapacitors. Here, a nucleotide‐tackified adhesive organohydrogel electrolyte is successfully constructed and exhibits freezing resistance and water‐holding ability based on the water/glycerol binary solvent system. Adenosine monophosphate enables the organohydrogels to possess outstanding adhesion and mechanical robustness. The robust adhesion can ensure close contact between the organohydrogel electrolyte and electrodes for constructing an all‐in‐one supercapacitor with low interfacial contact resistance. Impressively, the integrated organohydrogel‐based supercapacitors display an areal specific capacitance of 163.6 mF cm−2. Besides, the supercapacitors feature prominent environmental stability with capacitance retention of 90.6% after 5000 charging/discharging cycles at −20 °C. Furthermore, based on the strong interfacial adhesion, the supercapacitors present excellent electrochemical stability without delamination/displacement between electrolyte and electrodes even under severe deformations such as bending and twisting. It is anticipated that this work will provide an encouraging way for developing flexible energy storage devices with electrochemical stability and environmental adaptability.

Maintaining enough flexibility and satisfied electrochemical performance simultaneously at subzero temperatures is still challengeable for flexible solid supercapacitors. In the present work, by adopting an organohydrogel electrolyte and reduced graphene oxide (rGO) films with microvoids serving as electrodes, a supercapacitor, which could be steadily operated down to −60 °C, has been obtained and has shown excellent low-temperature tolerance. The organohydrogel electrolyte consists of LiCl in glycerol/water solution containing polyvinyl alcohol, exhibiting excellent flexibility at −60 °C. Due to the introduction of micropores between rGO sheets, the porous membrane can be folded even in liquid nitrogen. Combining the rGO electrodes with the organohydrogel electrolyte, the maximum voltage of the present supercapacitor could be extended to 2.0 V, and a capacitance of 7.73 F·g–1 at −60 °C could be achieved. After 5000 charge/discharge cycles at −20 °C, the capacitance retention rate is 87.5%. The excellent flexibility and low-temperature resistance of the current supercapacitor pave a novel way for developing compression-resistant electronic samples compatible with a low-temperature environment.