LAUSR

In carbon allotropes, interfacial engineering of various sp2 nanocarbon building blocks has shown great promise in designing and fabricating creative nanocarbon assemblies with novel structural and functional properties. Here, a robust, flexible, metal‐like heterostructured carbon nanotube (CNT) film formed of amorphous graphene nanosheets (AGNs) on CNT networked film is demonstrated, presenting a sp3‐sp2 dominated interfacial heterostructure. Extensive characterization reveals that AGN exhibits a complete absence of long‐range periodicity with twisty six‐member rings. Such 2D graphene mailed 1D CNT structure endows the heterostructured carbon nanocomposite film with a combination of unique properties, including surface nano‐flattening (flatness fourfold of the raw CNT film), excellent anti‐wear performance, greatly enhanced modulus (enhanced by 400%), hardness (enhanced by 300 times), and conductivity (enhanced by 270%). Unlike conventional carbon‐based materials, such flexible films show distinct substantial deformability and rapid resilience over wide temperatures (−196–≈1300 °C), which facilitate the design of new‐concept lightweight high‐temperature resistant and shape‐transformable materials for advanced aerospace applications under extreme conditions.