This work describes a simple, inexpensive, and robust method to prepare a flexible “all in one” integrated hydrogel supercapacitors (HySCs). Preparing smart hydrogels with high electrical conductivity, ability to stretch significantly, and excellent mechanical properties is the last challenge for tailored wearable devices. In this paper, we employed a physical crosslinking process that involves consecutive freezing and thawing cycles to prepare a polyvinyl alcohol (PVA)-based hydrogel. Exploiting the self-healing properties of these materials, the assembly of the different layers of the HySCs has been performed. The ionic conductivity within the electrolyte layer arises from the inclusion of an H₂SO₄ solution in the hydrogel network. Instead, the electronic conductivity is facilitated by the addition of the conductive polymer PANI-PAMPSA into the hydrogel layers. Electrochemical measures have highlighted newsworthy properties related to our HySCs, opening their use in wearable electronic applications.

This research study aims to explore the synergistic effects of incorporating polyvinylidene fluoride (PVDF) into polyvinyl alcohol (PVA) hydrogels to enhance their suitability for triboelectric sensors applications. The preparation process employs a method of freezing/thawing conducted in dimethyl sulfoxide (DMSO), followed by solvent replacement with water. This approach effectively preserves PVDF in its α phase, eliminating piezoelectric effects and enhancing the hydrogels’ mechanical properties. The use of DMSO contributes to reduced pore size, while incorporating PVDF significantly improves the three-dimensional network structure of the hydrogels, resulting in enhanced thermal and chemical resistance. Thorough characterization of the resulting PVA/PVDF composite hydrogels, prepared with varying ratios of PVA to PVDF (10:0, 8:2, and 5:5), was conducted by using scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), electrochemical impedance spectroscopy (EIS), rheology, and thermogravimetric analysis (TGA). Notably, the composite hydrogels were tested in pressure sensors and human voice sensors, demonstrating their capability to recognize different patterns associated with various letters. The incorporation of PVDF significantly enhanced the signal-to-noise ratio in PVA/PVDF-based sensors compared with those made solely from PVA, highlighting a notable improvement in voice detection. The enhancements were quantified as 56% for “a”, 35% for “r”, and 47% for “m”.