Electrochemical capacitors (ECs) provide appealing energy storage solutions, because of their higher power density, better safety and greater life span relative to lithium batteries. Rational design and synthesis of two-dimensional (2D) materials (such as graphene, MXene, transition metal dichalcogenides, etc.) has shown great impact for transformative technological advances for ECs. We will discuss the discovery of a 2D conductive supramolecular hybrid framework material, as well as its structure and relevant electrochemical properties for ECs. The 2D framework comprises periodically stacked 2D nanosheets with 1.2-nm basal spacing. In contrast to the pre-existing framework materials (for example MOFs), this conductive 2D framework has large density (~1.8 g cm−3) and low porosity (16.5 m2 g−1). The electrochemical performance (up to 732 F cm−3 in neutral aqueous electrolytes) and pseudocapacitive intercalation mechanism will be highlighted.