Many studies have been conducted to fabricate unique structures on flexible substrates and to apply such structures to a variety of fields. However, it is difficult to produce unique structures such as multilayer, nanospheres and porous patterns on a flexible substrate. We present a facile method of nanospheres based on laser-induced porous graphene (LIPG), by using laser-induced plasma (LIP). We fabricated these patterns from commercial polyimide (PI) film, with a 355 nm pulsed laser. For a simple one-step process, we used laser direct writing (LDW), under ambient conditions. We irradiated the PI film at a defocused plane −4 mm away from the focal plane, for high pulse overlap rate. The effect of the laser scanning speed was investigated by FE-SEM, to observe morphological characterization. Moreover, we confirmed the pattern characteristics by optical microscope, Raman spectroscopy and electrical experiments. The results suggested that we could modulate the conductivity and structural color by controlling the laser scanning speed. In this work, when the speed of the laser is 20 mm/s and the fluence is 5.28 mJ/cm2, the structural color is most outstanding. Furthermore, we applied these unique characteristics to various colorful patterns by controlling focal plane.