Nacre, a biological composite material derived from mollusk shells, exhibits exceptional mechanical properties surpassing those of its constituent phases due to its unique microstructure. It resembles a hierarchical brick-and-mortar structure, wherein approximately 95% of the volume fraction is occupied by brittle aragonite platelets, while the remaining 5% comprises a polymeric matrix of proteins and polysaccharides. Despite the minor volumetric contribution of this matrix to the overall composite structure, the resulting material exhibits a fracture toughness that surpasses that of pure aragonite by a factor of 3–9. Graphene nanoplatelets (GnPs) can be employed to create nacre-like structures due to their unique properties and ability to be oriented in a controlled manner. Numerous studies documented in the literature have sought to emulate Nacre's hierarchical architecture by subjecting graphene nanoplatelets to electric field-induced alignment. Furthermore, computational models have been developed to predict the resultant platelet spacing within such composites as a function of material parameters and applied voltage. In this study, a top-down approach was adopted to demonstrate that the spacing between the graphene platelets within a matrix can be used as a critical design parameter capable of influencing and optimizing the overall material properties of the composite. To achieve that, an existing computational model was modified to specify GnP separation as an input. An experimental approach was adopted to determine the requisite voltage and processing time using this desired separation. The preliminary data supports the feasibility of this approach for producing optimal results.