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The present study concerns codeposition of nanocrystalline aluminide particles (NbAl3 and Cu9Al4) along with electrodeposition of Cu on a Cu substrate. It is shown that the success of codeposition primarily depends on the selection of an appropriate electrolyte. Following codeposition under an optimum deposition condition, the microstructure, phase identity and composition of the deposit layer have been studied. In addition, microhardness and electrical resistivity of the deposit have been determined. A suitable correlation of the microstructure and composition of the deposit with its properties suggests that codeposition of NbAl3 is more effective in enhancing the hardness. However, codeposition beyond a limit adversely affects the electrical conductivity. The optimum conditions for codeposition to enhance hardness without adversely affecting conductivity have been determined. Finally, it is predicted codeposition could be a suitable technique for developing a surface composite microstructure with uniform distribution of nanocrystalline aluminide particles.