Presently disclosed is a multi-layered carbon-based scaffolded structure having a conductive substrate. A first film is deposited on the conductive substrate and includes: a first concentration of three-dimensional (3D) carbon-based particles comprising: a plurality of conductive 3D aggregates formed of graphene sheets that are sintered together to define a 3D hierarchical open porous structure with mesoscale structuring in combination with micron-scale fractal structuring that is also configured to provide conduction between contact points of the graphene sheets. A porous arrangement is formed in the 3D hierarchical open porous structure and contains a liquid electrolyte configured to provide ion transport through a plurality of interconnected porous channels. The first film is configured to provide a first conductivity. A second film is deposited on the first film and comprising a second concentration of 3D carbon-based particles. The second film configured to provide a second conductivity lower than the first conductivity.