Mechanical alloying (MA) has been and continues to be thoroughly examined for creating structural materials, but the production of catalysts is relatively rare. This is especially true for catalysts used in the production of carbon nanofibers (CNFs), a versatile material for applications such as energy storage, catalyst support, advanced composites and others. The application of MA to create CNFs presents a valuable tool in reducing their cost and complexity, and thereby may increase their commercial potential. In this study, the effects of milling duration on CNF deposition are studied by the complementary methods of X-ray diffraction, compositional mapping, electron microscopy, particle size analysis and surface area analysis. These were used to determine microstructural and macroscale evolution of the catalyst powder and its effects on the kinetics and characteristics of carbon deposition using Ni and Ni 30 at % Cu. The results have important implications for low cost catalyst production and provide general guidance on the development of catalytic materials in miscible systems.