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GaN-based light-emitting diodes (LEDs) with naturally textured surfaces grown by MOCVD were demonstrated. In this study, a growth-interruption step and a surface treatment using biscyclopentadienyl magnesium (CP2Mg) were simultaneously performed to form a plurality of nuclei sites on the surface of a p-type cladding layer, and then a p-type contact layer was grown on the p-type cladding layer, so as to create a p-type contact layer with a rough surface having truncated pyramids. Experimental results indicated that GaN-based LED with the truncated pyramids on the surface exhibited an enhancement in output power of 66% at 20 mA. It is worth noting that the typical 20-mA-driven forward voltage is only slightly higher than those of conventional LEDs (without the Mg-treatment process).