Nanocrystalline VC0.875 nonstoichiometric vanadium carbide powder has been prepared by high-energy milling. The crystal structure, microstructure, morphology, and particle size distribution of the starting and milled powders have been studied by X-ray diffraction, laser diffraction, and scanning electron microscopy. The particle size of the VC0.875 nanopowder has been calculated as a function of milling time in a model of the milling process. Comparison of experimental data and calculation results demonstrates that 10-h milling of vanadium carbide powder with an average particle size 6 μm yields nanopowder 40 to 80 nm in average particle size.