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GaN-based light-emitting diodes (LEDs) were grown on a patterned sapphire substrate (PSS) containing hemispheres on the growth surface. Free-standing LED structures were obtained by removing the PSS using laser lift-off technique. The N-face GaN surface with micron-sized concave hemisphere structures, which had been located between the sapphire and the GaN film, was then exposed and photo-electrochemically etched using a 2M KOH solution to create nano-sized pyramids. Aluminum was deposited on the roughened N-face GaN as a reflective layer. The roughened aluminum reflectors, consisting of micron-sized hemisphere structures and nano-sized pyramids, enhanced the light extraction efficiency through multiple scattering events of photons and randomized the directions of the photons. The subsequent enhancement in electroluminescence was 13% compared with an untextured control LED.