Surface texturing has been widely adopted to enhance the light extraction efficiency of light-emitting diodes (LEDs), and chemical etching is a technique commonly used to produce surface texturing. This study employed femtosecond lasers to apply ITO films directly onto the surface of LEDs to generate periodic micro/nanostructures and roughen the surface without contact or chemical substances. As a result, photons emitted in the active region escape into the free space, due to the scattering effect produced by texturing. This study discovered that light-emitting efficiency increases with surface roughness, and achieved an improvement of 18%. Caution regarding laser fluence was required during laser processing to avoid damaging the LED beneath the ITO film, which could detract from the electrical characteristics.