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Nanocrystalline diamond has been synthesized on a mirror-polished Si(001) substrate by means of direct ion beam deposition. Low-energy (80–200 eV) hydrocarbon and hydrogen ions, generated in a Kaufman ion source, were used to bombard the substrates. The bombarded samples were characterized by high-resolution transmission electron microscopy and Raman spectroscopy. Nanocrystalline diamond particles of random orientation were observed in a matrix of amorphous carbon film on the Si(001) substrate. The size of the nanocrystalline diamond particles varied in the range of 50–300 Å. The mechanism of ion-induced formation of nanocrystalline diamond is discussed.