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In the past decade, hydrogels have attracted growing interest for emerging applications in flexible electronic devices, human-machine interactions, energy supply, or energy storage. Developing a multifunctional gel architecture with superior ionic conductivity and good mechanical flexibility is a bottleneck to overcome. Herein, poly(vinyl alcohol)/sulfuric acid (PVA-H 2 SO 4 ) hydrogels were prepared via a freeze-thaw method. With the aim of tuning the formulation in view of a possible application in energy storage, the effects of different combinations in terms of the molecular weight (MW) of PVA and PVA-H 2 SO 4 weight ratio were investigated. Moreover, exploiting the self-healing properties of these hydrogels and the easy possibility of functionalizing them, i.e., introducing a conducting polymer such as poly(2-acrylamido-2-methyl-1-propane) sulfonic acid doped polyaniline (PANI_PAMPSA), a sandwiched all-in-one double-layer hydrogel (electrode/electrolyte configuration) was prepared (PVA-H 2 SO 4 -PANI_PAMPSA/PVA-H 2 SO 4 ). Results showed that the water content is independent of the PVA amount and MW; the polymer concentration has a significant effect on the formation of crystalline domains and therefore on swelling degree, whereas the cross-linking degree depends on the MW. The PVA MW has the maximum effect on the swelling percentage normalized with respect to the polymer fraction and the tensile properties of the hydrogel. The assembled all-in-one electrode/electrolyte shows promising ionic conductivity (439.7 mS cm -1 ) and specific capacitance performance (0.297 mF cm -2 at a current density of 0.025 mA cm -2 ), as well as excellent flexibility and considerable self-healing properties. These results will promote the development of self-healing symmetrical supercapacitors for storage devices in wearable electronics., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)