Nanocrystalline Sr2FeMoO6 films have been grown on a Si(100) substrate by pulsed laser deposition under different growth conditions including deposition temperature and time. A nanocrystalline single-phase Sr2FeMoO6 film was obtained at a temperature as low as 600 °C. This high-quality ferromagnetic film was found to have a saturation magnetic moment of 3.4μB per formula unit and a coercive field of 1.5 kOe at 77 K with micrometer-sized magnetic domains. By using glancing-incidence x-ray diffraction with different incident beam angles, the crystal structure of the film was sampled as a function of depth. For the as-grown Sr2FeMoO6 films thicker than 60 nm, a preferential orientation of the nanocrystals in the film was observed, despite the lack of good lattice matching with the Si substrate. At a higher deposition temperature of 800 °C, the as-grown film exhibited the same saturation magnetic moment but with a discernibly lower coercive field of 0.8 kOe, consistent with the larger grain size obtained at a higher growth temperature.