The carbon nanotube network decorated with Pt nanoparticles (PtCNT) irradiated by excimer laser as counter electrode (CE) of dye-sensitized solar cells (DSSCs) has been systematically demonstrated. The conversion efficiency would be improved from 7.12% to 9.28% with respect to conventional Pt-film one. It was attributed to the enhanced catalytic surface from Pt nanoparticles and the improved conductivity due to the adjoining phenomenon of PtCNTs irradiated by laser. Moreover, the laser annealing could also promote the interface contact between CE and conductive glass. Therefore, such a simple laser-irradiated PtCNT network is promising for the future flexible DSSCs applications.