A novel heteroepitaxial growth technique, quasi-van der Waals epitaxy, promises the ability to deposit three-dimensional GaAs materials on silicon using two-dimensional graphene as a buffer layer by overcoming the lattice and thermal expansion mismatch. In this study, density functional theory (DFT) simulations were performed to understand the interactions at the GaAs/graphene hetero-interface as well as the growth orientations of GaAs on graphene. To develop a better understanding of the molecular beam epitaxy-grown GaAs films on graphene, samples were characterized by x-ray diffraction (θ-2. θ scan, ω-scan, grazing incidence XRD and pole figure measurement) and transmission electron microscopy. The realizations of smooth GaAs films with a strong (111) oriented fiber-texture on graphene/silicon using this deposition technique are a milestone towards an eventual demonstration of the epitaxial growth of GaAs on silicon, which is necessary for integrated photonics application. ; School of Design