Nanofillers such as carbon fiber, carbon nanotube (CNT), 2D graphene, and hexagonal boron nitride are a proven reinforcement material at the microscale, leading to enhanced macroscopic property. [1][2][3] However, the augmentation of properties such as superior mechanical strength, increased electrical and thermal properties, and crack confinement in the material matrix is achieved only when the nanofillers are dispersed homogeneously. Until the advent of 2D graphene in 2004, [4,5] CNTs were the dominant nanofiller used in the synthesis of reinforced nanocomposites. CNT's high entanglement affinity, impurities, and challenges associated with processing hindered their application for novel composite materials development. [6][7][8] On the other hand, 2D graphene (Gr), whose material properties are comparable to CNTs, had many other novel physical, chemical, and electronic properties. Experimental and theoretical results boast that a single sheet of 2D graphene formed by the packing of carbon atoms into a honeycomb-like lattice is the strongest material developed to date. [9,10] The 2D graphene exhibits high modulus (%1 TPa), [11] tensile strength (%100 GPa), [11] superior thermal conductivity (3000-5000 W m À1 K À1 ), [12,13] exceptional electron mobility at room temperature (>200 000 cm 2 V À1 s À1 ), [14][15][16] and high transparency (97.7%) to incident light. [17,18] These outstanding physicochemical properties of 2D graphene make it a popular nanofiller for various applications, such as composite engineering materials, sensor, nanoelectronics, biomedical, and catalysis, to name a few. [19] Despite these excellent properties as a nanofiller, 2D graphene results in the aggregation or restacking of sheets due to strong π-π interaction. [20][21][22] Thus, formed nanocomposites exhibit poor mechanical (agglomerates form sites for stress concentration) and deteriorated electrochemical properties due to decreased active surface area. To fully exploit the outstanding properties of 2D graphene, various strategies have been used, such as crumbling the graphene sheets, adding spacers, and stacking 2D graphene into 3D hierarchical architecture. [23,24] Graphene material with 3D architecture, such as foam produced by chemical vapor deposition (CVD), has proved effective against agglomeration, unlike the 2D graphene flakes in the matrix material. The interconnected network of nodes and branches, which is characteristic of a 3D hierarchical structure of graphene foam (GrF), enables uninterrupted pathways to transfer electrons, phonons, and stresses, thus incorporating superior material properties in the reinforced matrix. [25][26][27] The porous 3D architecture in GrF offers low density (<5 mg cm À3 ), high surface area (%850 m 2 g À1 ), stable mechanical properties, accelerated electron and phonon transfer properties due to the reduced inter-sheet junction contact resistance, unlike the 2D graphene sheets.