Recent advancements in wearable electronic technology demand advanced power sources to be flexible, deformable, durable, and sustainable. An ionic-solution-modified conductive hydrogel-based triboelectric nanogenerator (TENG) has advantages in wearable devices. However, fabricating a conductive hydrogel with better mechanical and electrical properties is still a challenge. Herein, a simple approach is developed to insert ion-rich pores inside the hydrogel, followed by ionic solution soaking. The suggested ionic conductive hydrogel is obtained by cross-linking the polyvinyl alcohol (PVA) hydrogel and carboxymethyl cellulose sodium salt (CMC), followed by soaking in the ionic solution. Furthermore, a flexible and shape-adaptable single-electrode TENG (S-TENG) is fabricated by combinations of ionic-solution-modified dual-cross-linked CMC/PVA hydrogel and silicone rubber. Additionally, the effects of the CMC concentration, type of ionic solution, and concentration of optimized ionic solutions on the hydrogel properties and S-TENG output performance are studied systematically. The well-dispersed CMC- and PVA-based hydrogel provides ion-rich pores with high ion migration, leading to enhanced conductivity. The fabricated S-TENG delivers maximum output performance in terms of voltage, current, and charge density of ∼584 V, 25 μA, and 120 μC/m, respectively. The rectified S-TENG-generated energy is used to charge capacitors and to power a portable electronic display. In addition to energy harvesting, the S-TENG is successfully demonstrated as a touch sensor that can automatically control the light and the speaker based on human motions. This investigation provides a deep insight into the influence of the hydrogel on the device performance and gives a guidance for designing and fabrication of highly flexible and stretchable TENGs.