The recent development of dielectric microsphere lithography has been able to open up new means of performing simple and easy patterning on the semiconductor surfaces. Here, we report uniform and high-density arrays of microspheres using a solution-based spin-coating method. The arrays of microspheres were used for etching mask to form the arrays of III-nitride microrods. By regrowing GaN layer on the microrod structures, high-quality GaN layer was achieved in terms of surface morphology as well as XRD characterization. To apply the advantages such as improved crystal quality and light extraction enhancement, light-emitting diodes (LEDs) were grown and then fabricated. The regrown LEDs with microspheres showed much improved optical output power and forward voltage characteristics in the same current injection. Therefore, we believe that this approach is quite useful for the development of high efficiency LEDs for future lighting.