Graphene

Polymer nanocomposite

Engineering

Composite material

Thermal conductivity

Nanotechnology

Structural engineering

Nanocomposite

Composite number

Thermal conduction

Materials science

Finite element method

Hyperelastic material

Advanced Functional Materials

Graphene‐reinforced polymer composites with high thermal conductivity show attractive prospects as thermal transfer materials in many applications such as intelligent robotic skin. However, for the most reported composites, precise control of the thermal conductivity is not easily achieved, and the improvement efficiency is usually low. To effectively control the 3D thermal conductivity of graphene‐reinforced polymer nanocomposites, a hyperelastic double‐continuous network of graphene and sponge is developed. The structure (orientation, density) and thermal conductivity (in‐plane, cross‐plane) of the resulting composites can be effectively controlled by adjusting the preparation and deformation parameters (unidirectional, multidirectional) of the network. Based on the experimental and theoretical simulation results, the thermal conduction mechanism is summarized as a two‐stage transmission of phonons. The in‐plane thermal conductivity increases from 0.175 to 1.68 W m −1 K −1 when the directional compression r...

Efficiently Controlling the 3D Thermal Conductivity of a Polymer Nanocomposite via a Hyperelastic Double‐Continuous Network of Graphene and Sponge