La067Ba033MnO3 thin films were grown on LaAlO3 substrate using pulsed laser deposition. The microstructure, magnetic and electrical properties of as-grown, annealed and CO2-laser-irradiated （CLI） LBMO films were studied. It is found that, after laser irradiation, the enhancement of the crystallinity of the film is accompanied by the emergence of the plain-like surface morphology with smaller roughness. The structure and magneto-transport properties of LBMO films are markedly improved in several dozens of seconds via CO2 laser irradiation. Compared with the annealing treatment, laser irradiation is a fast and effective way to tailor CMR manganites for industrial applications.