In order to solve the problems of GaN heteroepitaxy on sapphire substrate, some techniques were explored. Freestanding GaN substrates have been made by hydride vapor phase epitaxy (HVPE), laser lift-off (LLO), and chemical mechanical polishing techniques. Wafer bending and cracking in the HVPE growth were partly settled by pulsed flow modulation method. High-crystal quality was established for 1.2 mm thick GaN substrate by X-ray diffraction measurement, in which the full width of half maximum values were 72, 110 arcsec for (102), (002) peaks. A novel micro-size patterned sapphire substrate (PSS) and a nano PSS were also fabricated. High-power vertical structure light emitting diodes (VSLEDs) have been developed by Au–Sn eutectic wafer bonding, homemade micro-area LLO, and light extraction structure preparation. The high-injection-level active region with low temperature GaN sandwiched layers was used for low-efficiency droop. The light output power of VSLED was achieved as 400 mW driven at 350 mA, and the dominant wavelength is about 460 nm. The structures and properties of strain modulated superlattices (SLs) and quantum wells as well as advanced simulation of carriers transport across the electron blocking layer were investigated in laser diodes. The hole concentration was achieved as high as 1.6 × 1018 cm−3 in AlGaN/GaN SLs:Mg by inserting an AlN layer. High-quality AlGaN epilayers and structures were grown by MOCVD. Some device structures of UV LEDs and detectors were demonstrated. The emission wavelength of 262 nm UV LED has been successfully fabricated. At last, high-quality InN and InGaN materials for solar cell were grown by boundary-temperature-controlled epitaxy and growth-temperature-controlled epitaxy. Hall-effect measurement showed a recorded electron mobility of 3,280 cm2/(V s) and a residual electron concentration of 1.47 × 1017 cm−3 at 300 K.