AbstractThis paper reports the atmospheric‐pressure MOVPE growth of In‐rich InAlN. All InAlN films prepared here (Al content:0∼ 0.43) do not show phase separation. The incorporation of Al in InAlN is decreased with increasing growth temperature. A decrease in Al content is also observed for films grown at a position farther from the up‐stream end of the susceptor. The marked decrease in the Al content along the gas flow direction seems to be caused by the shortage of TMA supply at the downstream by the parasitic reaction of TMA. A single‐crystalline InAlN film with an Al content of 0‐0.43 is successfully grown by adjusting growth temperature and TMA/(TMI+TMA) molar ratio. FWHM of X‐ray rocking curve for InAlN is increased with increasing Al content. The carrier concentrations in InAlN films are comparable to that in InN (1‐5 × 1019 cm–3). All the single‐crystalline InAlN films with an Al content of 0‐0.3 show a photoluminescence at room temperature. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)