Hidemi Kato

Crack‐free nanocellular graphenes are attractive materials with extraordinary mechanical and electrochemical properties, but their homogeneous synthesis on the centimeter scale is challenging. Here, a strong nanocellular graphene film achieved by the self‐organization of carbon atoms using liquid metal dealloying and employing a defect‐free amorphous precursor is reported. 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 × 10 4 S m −1 ). This unique material has excellent potential for flexible and high‐rate sodium‐ion battery applications.