Thin films of (001)-oriented Sr2FeMoO6 have been epitaxially deposited or LaAlO3 and SrTiO3 (001) substrates by pulsed laser deposition. The deposition conditions were optimized. Single-phase Sr2FeMoO6 was obtained in 100 mTorr 99.999% Ar gas at 825 degrees C. Transport and magnetic data showed a metallic temperature dependence and a saturation magnetization M-s at 10 K of 3.2 mu(B)/f.u. However, the Curie temperature T(C)approximate to 380 K was reduced from 415 K found for tetragonal polycrystalline best ceramics, which lowers M-s at 300 K in the thin films to 1.5 mu(B)/f.u. compared to 2.2 mu(B)/f.u. in the ceramics. A low remanence was attributed to the presence of antiphase boundaries. A Wheatstone bridge arrangement straddling a bicrystal boundary was used to verify that spin-dependent electron transfer through a grain boundary and not an antiphase boundary is responsible for the low-field magnetoresistance found in polycrystalline samples below T-C. (C) 2000 American Institute of Physics. [S0021-8979(00)55908-8].