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Silicon oxide films containing nanocrystalline silicon (nc-SiOx:H) are deposited by co-sputtering technology at low temperatures (<400°C) that are much lower than the typical growth temperature of nc-Si in SiO2. The microstructures and bonding properties are characterized by Raman and FTIR. It is proven that an optimum range of substrate temperatures for the deposition of nc-SiOx:H films is 200–400°C, in which the ratio of transition crystalline silicon decreases, the crystalline fraction is higher, and the hydrogen content is lower. The underlying mechanism is explained by a competitive process between nc-Si Wolmer–Weber growth and oxidation reaction, both of which achieve a balance in the range of 200–400°C. We further implement this technique in the fabrication of multilayered nc-SiOx:H/a-SiOx:H films, which exhibit controllable nc-Si sizes with high crystallization quality. [ABSTRACT FROM AUTHOR]