Multifunctionality through Embedding Patterned Nanostructures in High‐Performance Composites

Abstract Despite being a pillar of high‐performance materials in industry, manufacturing carbon fiber composites with simultaneously enhanced multifunctionality and structural properties has remained elusive due to the lack of practical bottom‐up approaches with control over nanoscale interactions. Guided by the droplet's internal currents and amphiphilicity of nanomaterials, herein, a programmable spray coating is introduced for the deposition of multiple nanomaterials with tailorable patterns in composite. It is shown that such patterns regulate the formation of interfaces, damage containment, and electrical‐thermal conductivity of the composites, which is absent in conventional manufacturing that primarily rely on incorporating nanomaterials to achieve specific functionalities. Molecular dynamics simulations show that increasing the hydrophilicity of the hybrid nanomaterials, which is synchronous with shifting patterns from disk to ring, improves the interactions between the carbon surfaces and epoxy at the interfaces,manifested in enhanced interlaminar and flexural performance. Transitioning from ring to disk creates a larger interconnected network leading to improved thermal and electrical properties without penalty in mechanical properties. This novel approach introduces a new design , where the mechanical and multifunctional performance is controlled by the shape of the deposited patterns, thus eliminating the trade‐off between properties that are considered paradoxical in today's manufacturing of hierarchical composites.