Crack-free nanocellular graphenes are attractive materials with extraordinary mechanical and electrochemical properties, but their homogeneous synthesis on the centimeter scale is challenging. Here, we report a strong nanocellular graphene film achieved by the self-organization of carbon atoms using liquid metal dealloying and employing a defect-free amorphous precursor. This study demonstrates that a Bi melt strongly catalyzes the self-structuring of graphene layers at low processing temperatures. The robust nanoarchitectured graphene displays a high-genus seamless framework and exhibits remarkable tensile strength (34.8 MPa) and high electrical conductivity (1.6 × 104 S/m). This unique material has excellent potential for flexible and high-rate sodium-ion battery applications.