Graphene is a key material of interest for modification of physicochemical surface properties. However, its flat surface is a limitation for applications requiring a high specific surface area. This restriction may be overcome by integrating 2D materials in a 3D structure. Here, a strategy for the controlled synthesis of Graphene-Mesoporous Germanium (Gr-MP-Ge) nanomaterials is presented. Bipolar electrochemical etching and chemical vapor infiltration were employed for, respectively, nanostructuration of Ge substrate and subsequent 3D nanographene coating. While Raman spectroscopy reveals tunable domain size of nanographene with the treatment temperature, transmission electron microscopy data confirm that the crystallinity of Gr-MP-Ge is preserved. X-ray photoelectron spectroscopy indicates the non-covalent bonding of carbon to Ge for Gr-MP-Ge. State-of-the-art molecular dynamics modeling allows for a deeper understanding of the synthesis process through the presence of radicals. The successful synthesis of this nanomaterials offers integration of nanographene into a 3D structure with a high aspect ratio and light weight, thereby opens avenues to a variety of applications for this versatile nanomaterial.