Robust and Versatile Heterostructured Carbon Nanocomposites with Diverse Adaptability to Harsh Environments

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.