Exciting progress has been made in the use of graphene for bio- and chemical sensing applications. In this regard, interfacing lipid membranes with graphene provides a high-sealing interface that is resistant to nonspecific protein adsorption and suitable for measuring biomembrane-associated interactions. However, a controllable method to form well-defined lipid bilayer coatings remains elusive, and there are varying results in the literature. Herein, we demonstrate how design strategies based on molecular self-assembly and surface chemistry can be employed to coat graphene surface with different classes of lipid membrane architectures. We characterize the self-assembly of lipid membranes on CVD-graphene using quartz crystal microbalance with dissipation, field-effect transistor, and Raman spectroscopy. By employing the solvent-assisted lipid bilayer (SALB) method, a lipid monolayer and bilayer were formed on pristine and oxygen-plasma-treated CVD-graphene, respectively. On these surfaces, vesicle fusion method resulted in formation of a lipid monolayer and intact vesicle layer, respectively. Collectively, these findings provide the basis for improved surface functionalization strategies on graphene toward bioelectronic applications.