Wurtzite InN films were prepared on a 6H-SiC substrate by a self-designed plasma-assisted metal-organic molecular-beam epitaxy system without a buffer layer. In this article, the authors investigate the structural and optical properties of InN films grown on a 6H-SiC substrate. The crystallinity and microstructure of the thin film were further characterized by x-ray diffraction (XRD), field-emission scanning-electron microscopy, and transmission-electron microscopy. Electrical and optical properties were evaluated by Hall and photoluminescence (PL) measurements. XRD results indicate that InN film grown at 500 °C is epitaxially grown along the c-axis orientation. The two-dimensional growth mode is clearly shown in scanning-electron microscope images. Room-temperature PL spectra show that the emission peak is located at ∼0.83 eV due to the Burstein–Moss effect. In addition, the crystalline InN samples crack and peel away from the substrate at elevated growth temperature. This phenomenon may be attributed to lattice mismatch and grain coalescence while increasing the growth temperature. The narrow window of the growth temperature plays an important role in engineering the InN epitaxial growth.