Carbon structures are commonly used as the reinforcement phase in composite materials toimprove the electrical, mechanical, and/or thermal properties of the matrix material. The structural diversity of carbon in its various forms (graphene, carbon nanotubes, graphite fibers, for example) makes it a useful reinforcement phase, as the properties of the composite material can be tailored for a specific application depending on the structure and properties of the carbon structure used. In this work, the incorporation of graphene/graphitic carbon into an aluminum metal matrix by an electrocharging assisted process (EAP) was investigated to create a composite material with enhanced electrical conductivity and yield strength. The increased electrical conductivity makes the composite suitable for application in more efficient power transmission lines. The increased strength makes it useful as a lightweight structural material in aerospace applications. The EAP involves applying a direct current to a mixture of molten aluminum and activated carbon to induce the crystallization of graphitic sheets/ribbons that extend throughout the matrix. The effect of processing conditions (current density, in particular) on the graphitic carbon structure, electrical properties, and mechanical properties of the composite material was investigated. The effect of porosity/voids and oxide formation was discussed with respect to the measured properties, and updates to the EAP system were made to mitigate their detrimental effects. It was found that the application of current results in some increase in graphitic carbon crystallite size calculated from Raman spectra, but many areas show the same crystallite size as the activated carbon starting material. It is likely that the current density used during processing was too low to see significant crystallization of graphitic carbon. There was no increase in electrical conductivity compared to a baseline sample with no added carbon, most likely due to porosity/voids in the samples. The mechanical characterization results indicated that the graphitic carbon clusters formed by the process did not act as an effective reinforcement phase, with no improvement in hardness and a decrease in elastic modulus measured by nanoindentation. The decreased elastic modulus was a result of compliant carbon clusters and porosity in the covetic samples. The porosity/voids were not entirely eliminated by the updates to the system, thus the electrical conductivity still did not improve. Additionally, a multifunctional composite structure consisting of a carbon-fiber reinforced polymer (CFRP) laminate with added copper mesh layers was investigated for use in aerospace applications as a structural and electromagnetic interference (EMI) shielding component. The CFRP provides primarily a structural function, while the copper mesh layers were added to increase EMI shielding effectiveness (SE). Nanoindentation was used to study the interfacial mechanical properties of the fiber/polymer and Cu/polymer interfaces, as the interfacial strength dictates the overall mechanical performance of the composite. Further, a finite element model of EMI SE was made to predict SE in the radiofrequency to microwave range for different geometry and configurations of the multifunctional composite structure. The model was used to help determine the optimum design of the multifunctional composite structure for effective shielding of EM radiation. It was found from nanoindentation near the fiber/polymer and Cu/polymer interfaces that the carbon fibers act as an effective reinforcement phase with hardness in the matrix increasing in the interphase region near the carbon fibers due to strong interfacial adhesion. In contrast, the Cu/polymer interface did not exhibit an increase in hardness, indicating poor interfacial adhesion. The EMI SE model indicated that the combination of CFRP layers, which primarily shields EMI by absorption, and Cu mesh, which predominantly shields by reflection, provided adequate SE over a wider frequency range than the individual components alone. Further, it was found that the SE of the CFRP layers were improved by including multiple plies with different relative fiber orientations.