A novel carbon nanotube-patterned sapphire substrate (CPSS) has been utilized for the growth of GaN material and fabrication of a InGaN/GaN light emitting diode (LED) by metal–organic vapor phase epitaxy. Different lateral strain distributions and stress reductions were observed in a GaN thin film on CPSS compared with those on a conventional sapphire substrate. Nanoheteroepitaxy induced by small size nucleation islands of about 50 nm is ascribed to this significant strain modulation. The crystalline quality of the GaN thin film was also improved, as illustrated by X-ray diffraction. Performances of 1 mm × 1 mm LEDs on CPSS were also enhanced, with an operational power increase of 37.5% and higher saturation current.