Three-dimensional (3D) macroporous graphene foam based multifunctional epoxy composites are developed in this study. Facile dip-coating and mold-casting techniques are employed to engineer microstructures with tailorable thermal, mechanical, and electrical properties. These processing techniques allow capillarity-induced equilibrium filling of graphene foam branches, creating epoxy/graphene interfaces with minimal separation. Addition of 2 wt % graphene foam enhances the glass transition temperature of epoxy from 106 to 162 °C, improving the thermal stability of the polymer composite. Graphene foam aids in load-bearing, increasing the ultimate tensile strength by 12% by merely 0.13 wt % graphene foam in an epoxy matrix. Digital image correlation (DIC) analysis revealed that the graphene foam cells restrict and confine the deformation of the polymer matrix, thereby enhancing the load-bearing capability of the composite. Addition of 0.6 wt % graphene foam also enhances the flexural strength of the pure epoxy by 10%. A 3D network of graphene branches is found to suppress and deflect the cracks, arresting mechanical failure. Dynamic mechanical analysis (DMA) of the composites demonstrated their vibration damping capability, as the loss tangent (tan δ) jumps from 0.1 for the pure epoxy to 0.24 for ∼2 wt % graphene foam-epoxy composite. Graphene foam branches also provide seamless pathways for electron transfer, which induces electrical conductivity exceeding 450 S/m in an otherwise insulator epoxy matrix. The epoxy-graphene foam composite exhibits a gauge factor as high as 4.1, which is twice the typical gauge factor for the most common metals. Simultaneous improvement in thermal, mechanical, and electrical properties of epoxy due to 3D graphene foam makes epoxy-graphene foam composite a promising lightweight and multifunctional material for aiding load-bearing, electrical transport, and motion sensing in aerospace, automotive, robotics, and smart device structures.

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