Highly conductive SrMoO3 thin films with good crystallinity and smooth surface were grown on SrTiO3 (0 0 1) substrates by pulsed laser deposition. The effects of substrate temperature and oxygen pressure on the structure, surface morphology, and electrical properties were studied. In the range of substrate temperatures from 560 degreesC to 640 degreesC and oxygen pressure from 10 (-3) to 10 (-4) Pa studied in our experiments, high-quality SrMoO3 thin films were produced. Beyond the top temperature or oxygen pressure limit, SrMoO4 appears as an impurity phase. High-resolution transmission electron microscopy (HRTEM) study shows that the SrMoO3 film has high-quality crystallinity and an epitaxial nature. The root-mean-square surface roughness of the film deposited at 2.5 x 10 (-4) Pa is 3.9 Angstrom. The films exhibit metallic conduction, which results from the delocalized electrons from Mo. X-ray photoelectron spectroscopy (XPS) measurements characterized its core level spectra and the valence band.