The development of robust electrochemical energy storage devices, exhibiting fast charge storage kinetics and high Coulombic efficiency over multiple operation cycles, is an ongoing technological challenge. Aqueous electrical double-layer capacitors (supercapacitors) using carbon-based materials are considered to be a highly promising and environmentally sustainable option for the energy storage grid . However, the energy density of traditional supercapacitors is low due to the mechanism of the overall charge storage process, which involves the reversible non-Faradaic physisorption of ions inside the electrical double layer (EDL) . Enhancing the capacitance of supercapacitors is therefore crucial to improving the energy density of such devices. Graphene possesses a high surface area (2630 m 2 g -1 for monolayer graphene) compared to amorphous carbon, that can be utilized for the accumulation of ions within the EDL and thus significantly increase the capacitance of the electrodes. However, the successful utilization of the electrochemically active surface area of the electrode is directly related to its accessibility by the electrolyte (e.g., ingress of the electrolyte into its porous structure). On this basis, understanding the mechanism of wetting at the carbon/aqueous electrolyte interface under potential bias (the phenomenon of electrowetting ) is essential in the pursuit of strategies to enhance the capacitance of the devices .