A three-dimensional holey graphene framework (HGF) is introduced as a high-performance binder-free supercapacitor electrode with exceptional electrochemical properties. The HGF exhibits a high gravimetric capacitance of 298 F g⁻¹ and a high volumetric capacitance of 212 F cm⁻³ in organic electrolytes, achieving energy densities of 35 Wh kg⁻¹ and 49 Wh l⁻¹, which are comparable to those of lead acid batteries. The HGF's unique structure, with a hierarchical porous network and high packing density, enables efficient ion transport and access to a large surface area, resulting in high energy and power densities. The HGF electrode demonstrates excellent electrochemical stability, retaining 95% of its capacitance after 20,000 cycles at high current densities. The HGF also shows superior performance in both aqueous and organic electrolytes, with a gravimetric capacitance of 298 F g⁻¹ in organic electrolytes, leading to an unprecedented gravimetric energy density of 127 Wh kg⁻¹. The HGF-based supercapacitor achieves a high energy density of 35.1 Wh kg⁻¹ and 49.2 Wh l⁻¹ when fully packaged, surpassing commercial activated carbon-based supercapacitors. The HGF's unique hierarchical porosity and high ion accessibility enable efficient ion transport and high rate capability, making it a promising material for high-performance energy storage applications.A three-dimensional holey graphene framework (HGF) is introduced as a high-performance binder-free supercapacitor electrode with exceptional electrochemical properties. The HGF exhibits a high gravimetric capacitance of 298 F g⁻¹ and a high volumetric capacitance of 212 F cm⁻³ in organic electrolytes, achieving energy densities of 35 Wh kg⁻¹ and 49 Wh l⁻¹, which are comparable to those of lead acid batteries. The HGF's unique structure, with a hierarchical porous network and high packing density, enables efficient ion transport and access to a large surface area, resulting in high energy and power densities. The HGF electrode demonstrates excellent electrochemical stability, retaining 95% of its capacitance after 20,000 cycles at high current densities. The HGF also shows superior performance in both aqueous and organic electrolytes, with a gravimetric capacitance of 298 F g⁻¹ in organic electrolytes, leading to an unprecedented gravimetric energy density of 127 Wh kg⁻¹. The HGF-based supercapacitor achieves a high energy density of 35.1 Wh kg⁻¹ and 49.2 Wh l⁻¹ when fully packaged, surpassing commercial activated carbon-based supercapacitors. The HGF's unique hierarchical porosity and high ion accessibility enable efficient ion transport and high rate capability, making it a promising material for high-performance energy storage applications.