The nanoscale electrical double layer plays a crucial role in macroscopic ion adsorption and reaction kinetics. In this study, we achieve controllable ion migration by dynamically regulating asymmetric electrical double layer formation. This tailors the ionic-electronic coupling interface, leading to the development of triboiontronics. Controlling the charge-collecting layer coverage on dielectric substrates allows for charge collection and adjustment of the substrate-liquid contact electrification property. By dynamically managing the asymmetric electrical double layer formation between the dielectric substrate and liquids, we develop a direct-current triboiontronic nanogenerator. This nanogenerator produces a transferred charge density of 412.54 mC/m