The outstanding demonstration of quantum confinement in Si nanocrystals (Si NC) in a SiC matrix requires the fabrication of Si NC with a narrow size distribution. It is understood without controversy that this fabrication is a difficult exercise and that a multilayer (ML) structure is suitable for such fabrication only in a narrow parameter range. This parameter range is sought by varying both the stoichiometric SiC barrier thickness and the Si-rich SiC well thickness between 3 and 9 nm and comparing them to single layers (SL). The samples processed for this investigation were deposited by plasma-enhanced chemical vapor deposition (PECVD) and subsequently subjected to thermal annealing at 1000-1100 degrees C for crystal formation. Bulk information about the entire sample area and depth were obtained by structural and optical characterization methods: information about the mean Si NC size was determined from grazing incidence X-ray diffraction (GIXRD) measurements. Fourier-transform infrared spectroscopy (FTIR) was applied to gain insight into the structure of the Si-C network, and spectrophotometry measurements were performed to investigate the absorption coefficient and to estimate the bandgap E-04. All measurements showed that the influence of the ML structure on the Si NC size, on the Si-C network and on the absorption properties is subordinate to the influence of the overall Si content in the samples, which we identified as the key parameter for the structural and optical properties. We attribute this behavior to interdiffusion of the barrier and well layers. Because the produced Si NC are within the target size range of 2-4 nm for all layer thickness variations, we propose to use the Si content to adjust the Si NC size in future experiments. (C) 2015 Elsevier B.V. All rights reserved.