Monocrystalline GaN(0001) thin films, void of oriented domain structures and associated low‐angle grain boundaries, have been grown via organometallic vapor phase epitaxy (OMVPE) on high‐temperature monocrystalline AlN(0001) buffer layers predeposited on vicinal &agr;(6H)–SiC(0001) wafers using TEG, TEA, and ammonia in a cold wall, vertical, pancake‐style reactor. The surface morphology was smooth, and the PL spectrum showed strong near‐band‐edge emission with a full width at half‐maximum (FWHM) value of 4 meV. The dislocation density within the first 0.5 &mgr;m was ≊1×109cm−2; it decreased substantially with increasing film thickness. Controlledn‐type Si doping of GaN has been achieved for net carrier concentrations ranging from ∼1×1017to 1×1020cm−3. Double‐crystal XRC measurements indicated a FWHM value of 66 arcsec for the GaN(0004) reflection. ©1995 American Institute of Physics.