Thick (up to 1 mm) AlN-SiC alloy crystals were grown on off-axis Si-face 6H-SiC (0001) substrates by the sublimation-recondensation method from a mixture of AlN and SiC powders at 1860–1990 °C in a N2 atmosphere. The color of the crystals changed from clear to dark green with increasing growth temperature. Raman spectroscopy and x-ray diffraction (XRD) confirmed an AlN-SiC alloy was formed with the wurtzite structure and good homogeneity. Three broad peaks were detected in the Raman spectra, with one of those related to an AlN-like and another one to a SiC-like mode, both shifted relative to their usual positions in the binary compounds, and the third broad peak with possible contributions from both AlN and SiC. Scanning Auger microanalysis (SAM) and electron probe microanalysis (EPMA) demonstrated the alloy crystals had an approximate composition of (AlN)0.75(SiC)0.25 with a stoi chiometric ratio of Al:N and Si:C. The substrate mi sorientati on ensured a two-dimensional growth mode confirmed by scanning electron microscopy (SEM).