Small-scale and high-performance energy storage devices have drawn tremendous attention with their portable, lightweight, and multi-functionalized features. Here, we present a foldable supercapacitor with affordable flexibility by adopting a developed design and electrode material system as a way to extend usability. Notably, to resolve the limited energy density of conventional capacitors, we successfully synthesize the CoO/NiCo-layered double hydroxide (LDH) core–shell nanostructure on Ni framework as a cathode material. Further, glucose-based activated carbon (GBAC) is utilized for the anode. The CoO/NiCo-LDH electrodes exhibited a high specific capacitance of ∼284.8 mAh g−1 at 1 A g−1, and GBAC delivers a high specific capacitance of ∼166 F g−1 at 1 A g−1. In the following, the combinatorial integration of these materials enabled the asymmetric supercapacitor (ASC) to increase the energy density by enhancing the capacitance and the voltage window, in which a hydrogel-based electrolyte was facilitated for the foldable and wearable capability. The energy density of the ASC device was ∼24.9 Wh kg−1 at a power density of ∼779.5 W kg−1 with a voltage window of ∼1.6 V. As demonstrated, a self-powered energy source was demonstrated by a serially connected multi-ASC device with a help of a commercial solar cell, which was employed for powering wearable healthcare monitoring devices, including personal alarms for patients and recording the human body’s electrical signals. The present work offers a viable approach to preparing potential candidates for high-performance electrodes of supercapacitors with deformable configurations to extend the powering capability of other electronic devices with physical functionalities used in wearable electronics.