Raman microscopy has been used to study the carrier concentration and mobility in n‐doped 3C‐SiC epilayers grown on different silicon substrates, namely (100) Si and (111) Si on axis and off‐axis towards the [110] direction. By analyzing the longitudinal optical phonon‐plasmon coupled mode (LOPC), we were able to estimate the 3C‐SiC electron bulk mobility (μ) within the range between 5 and 500 cm2/Vs. The carrier concentration (n) was ranging from 2×1016 to 6×1018 cm−3. The observed trend shows a reduction in the electron mobility as the carrier concentration increases for films grown on any substrate considered, accordingly to the existent theory. For equal values of doping concentration, 3C‐SiC epitaxial films grown on (100) Si substrates show a higher mobility than films grown on (111) Si counterparts. This could be ascribed to a higher defect density in (111) Si samples. A deeper characterization …