This study presents a novel approach to triboiontronics by dynamically controlling the formation of electrical double layers (EDLs) between dielectric substrates and liquids. The research demonstrates that by regulating the asymmetric formation of EDLs, it is possible to achieve controllable ion migration, which enhances the ionic-electronic coupling interface. This leads to the development of a direct-current triboiontronic nanogenerator (PDC-TING) that produces a transferred charge density of 412.54 mC/m², significantly exceeding that of current hydrovoltaic technology and conventional triboelectric nanogenerators. Incorporating redox reactions further enhances performance, resulting in a peak power density of 38.64 W/m² and a transferred charge density of 540.70 mC/m², demonstrating the potential of this technology for energy conversion and information flow. The study highlights the importance of the EDL in various chemical, biological, and environmental processes. It discusses the evolution of EDL models from the initial flat model of Helmholtz to the more complex Stern model, which accounts for the diffuse layer and the influence of solvation and ion size. The two-step model, which considers electron transfer and ionization reactions, is proposed for insulating dielectric-liquid interfaces, enabling the formation of an IHP and OHP. The research explores the effects of various factors on the performance of the PDC-TING, including the sputtering time of the metal layer, the hydrophilicity of the substrate, and the ion concentration in the liquid. It shows that increasing the ion concentration in the liquid can significantly improve the ion concentration gradient and reduce internal resistance, thereby enhancing the output of the PDC-TING. The study also demonstrates that the synergistic effect of dynamically controlling EDL formation and redox reactions can lead to the development of a more efficient triboiontronic device, the SDC-TING, which achieves a peak power density of 38.64 W/m² and a transferred charge density of 540.70 mC/m². The results show that the PDC-TING and SDC-TING have several orders of magnitude higher transferred charge density compared to hydrovoltaic technology and conventional TENGs. These devices have significant potential for applications in energy harvesting, storage, and information flow, including the development of bionic neurologic circuits for human-computer interaction and neuromorphic computing. The study also highlights the importance of dynamically controlling EDL formation for creating a tunable ionic-electronic coupling interface, which can facilitate in-depth studies of iontronics.This study presents a novel approach to triboiontronics by dynamically controlling the formation of electrical double layers (EDLs) between dielectric substrates and liquids. The research demonstrates that by regulating the asymmetric formation of EDLs, it is possible to achieve controllable ion migration, which enhances the ionic-electronic coupling interface. This leads to the development of a direct-current triboiontronic nanogenerator (PDC-TING) that produces a transferred charge density of 412.54 mC/m², significantly exceeding that of current hydrovoltaic technology and conventional triboelectric nanogenerators. Incorporating redox reactions further enhances performance, resulting in a peak power density of 38.64 W/m² and a transferred charge density of 540.70 mC/m², demonstrating the potential of this technology for energy conversion and information flow. The study highlights the importance of the EDL in various chemical, biological, and environmental processes. It discusses the evolution of EDL models from the initial flat model of Helmholtz to the more complex Stern model, which accounts for the diffuse layer and the influence of solvation and ion size. The two-step model, which considers electron transfer and ionization reactions, is proposed for insulating dielectric-liquid interfaces, enabling the formation of an IHP and OHP. The research explores the effects of various factors on the performance of the PDC-TING, including the sputtering time of the metal layer, the hydrophilicity of the substrate, and the ion concentration in the liquid. It shows that increasing the ion concentration in the liquid can significantly improve the ion concentration gradient and reduce internal resistance, thereby enhancing the output of the PDC-TING. The study also demonstrates that the synergistic effect of dynamically controlling EDL formation and redox reactions can lead to the development of a more efficient triboiontronic device, the SDC-TING, which achieves a peak power density of 38.64 W/m² and a transferred charge density of 540.70 mC/m². The results show that the PDC-TING and SDC-TING have several orders of magnitude higher transferred charge density compared to hydrovoltaic technology and conventional TENGs. These devices have significant potential for applications in energy harvesting, storage, and information flow, including the development of bionic neurologic circuits for human-computer interaction and neuromorphic computing. The study also highlights the importance of dynamically controlling EDL formation for creating a tunable ionic-electronic coupling interface, which can facilitate in-depth studies of iontronics.