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Vertically aligned single-crystalline silicon nanocone (Si-NC) arrays are grown on nickel-coated silicon (100) substrates by a novel method i.e., abnormal glow-discharge plasma sputtering reaction deposition. The experimental results show that the inlet / ratio has great effects on the morphology of the grown Si-NC arrays. The characterization of the morphology, crystalline structure and composition of the grown Si-NCs indicates that the Si-NCs are grown epitaxially in the vapor–liquid–solid mode. The analyses of optical emission spectra further reveal that the inlet methane can promote the growth of Si-NCs by raising the plasma temperature and enhancing the ion-sputtering. The understanding of the growth mechanism of the Si-NC arrays will be helpful for fabrication of required Si-NC arrays.