The multiple micro/nano-patterning on p-GaN surface by femtosecond (fs) laser irradiation through a micro-ball lens array (MBLA) mask has been established to improve the light extraction efficiency of GaN-based light-emitting diodes (LEDs). This technique was meant for the high-speed surface micro/nano-patterning of a p-GaN surface on a large area using fs laser irradiation. Compared with conventional LEDs with flat surfaces, dual-scale roughened structures on p-GaN surface LEDs used in the present experiment scatter and increase the effective critical angle, increasing the escape probability of photons. The relationship of the hole size on p-GaN surface and the refractive index of the MBLA material would be also discussed. With an injection current of 20 mA, the output power of the experimental LEDs markedly improved by a magnitude of 48% compared with conventional GaN-based LEDs.