The work aims to improve surface wettability and adsorbability of polyphenylene sulfide (PPS). Two commonly lasers, i.e., 355 nm (wavelength) pulsed ultraviolet (UV) laser and 1064 nm (wavelength) pulsed infrared (IR) fiber laser, were used to modify PPS surface. The effects of laser energy density on chemical composition of modified PPS surface were discussed. After PPS was modified by the two lasers under certain energy density, new groups such as C=O, COO—, —SO, —SO2 and —SO4 were detected in the method of X-ray photoelectron spectroscopy (XPS), this was probably since chemical bond ruptured and reacted with oxygen-containing species in the air. It was also found that relative content variation degree of chemical composition on the modified PPS surfaces increased with energy density. However, interaction mechanisms between the two lasers and PPS were different, hence variation degree of chemical composition on the PPS surface modified by pulsed UV laser was higher than that on the PPS surface modified by pulsed IR fiber laser under the same energy density. Chemical composition of PPS surfaces will change after surface modification by pulsed UV laser and pulsed IR fiber laser under certain energy density.