A thin, chemically inert 3C-SiC layer between GaN and Si helps not only to avoid the “melt-back” effect, but also to inhibit the crack generation in the grown GaN layers. The quality of GaN layer is heavily dependent on the unique properties of the available 3C-SiC/Si templates. In this paper, the parameters influencing the roughness, crystalline quality, and wafer bow are investigated and engineered to obtain high quality, low roughness 3C-SiC/Si templates suitable for subsequent GaN growth and device processing. Kinetic surface roughening and SiC growth mechanisms, which depend on both deposition temperature and off-cut angle, are reported for heteroepitaxial growth of 3C-SiC on Si substrates. The narrower terrace width on 4° off-axis Si enhances the step-flow growth at 1200 °C, with the roughness of 3C-SiC remaining constant with increasing thickness, corresponding to a scaling exponent of zero. Crack-free 3C-SiC grown on 150-mm Si substrate with a wafer bow of less than 20 μm was achieved. Both concave and convex wafer bow can be obtained by in situ tuning of the deposited SiC layer thicknesses. The 3C-SiC grown on off-axis Si, compared to that grown on on-axis Si, has lower surface roughness, better crystallinity, and smaller bow magnitude.