The polytype and surface and defect microstructure of epitaxial layers grown on 4H(1120), 4H(0001) on-axis, 4H(0001) 8°off-axis, and 6H(0001) on-axis substrates have been investigated. High-resolution x-ray diffraction (XRD) revealed the epitaxial layers on 4H(1120) and 4H(0001) 8°off-axis to have the 4H-SiC (silicon carbide) polytype, while the 3C-SiC polytype was identified for epitaxial layers on 4H(0001) and 6H(0001) on-axis substrates. Cathodoluminescence (CL), Raman spectroscopy, and transmission electron microscopy (TEM) confirmed these results. The epitaxial surface of 4H(1120) films was specular with a roughness of 0.16-nm root-mean-square (RMS), in contrast to the surfaces of the other epitaxial layer-substrate orientations, which contained curvilinear boundaries, growth pits (~3 · 10 4 cm )2 ), triangular defects >100 lm, and significant step bunching. Molten KOH etching revealed large defect densities within 4H(1120) films that decreased with film thickness tõ 10 6 cm )2 at 2.5 lm, while cross-sectional TEM studies showed areas free of defects and an indistinguishable film-substrate interface for 4H(1120) epitaxial layers.