Metal-modulated epitaxy allows controlled atomic layer-by-layer growth of thin films with almost ideal characteristics enabled by strain relaxation at the first atomic layer. The crystal's lattice structures match up, resembling a perfect crystal, with corresponding luminosity. The crystal had indium content ranging from x ∼ 0.22 to 0.67. Significant improvement in the crystalline quality and optical properties began at x ∼ 0.6. Films were grown at ∼400 °C to facilitate indium incorporation and with precursor modulation to enhance surface morphology and metal adlayer diffusion. These findings should contribute to the development of growth techniques for nitride semiconductors under high lattice misfit conditions.