Thin films of (001)-oriented Sr2FeMoO6 have been epitaxially deposited on LaAlO3 and SrTiO3 (001) substrates. Comparison of their transport and magnetic properties with those of polycrystalline ceramic samples shows a metallic versus semiconductor temperature dependence and a saturation magnetization M-s at 10 K of 3.2 mu(B)/f.u. in the film as against 3.0 for a tetragonal polycrystalline sample. However, the Curie temperature T(C)approximate to 389 K is reduced from 415 K found for the tetragonal ceramic, which lowers M-s at 300 K in the thin films to 2.0 mu(B)/f.u. compared to 2.2 mu(B)/f.u. in the ceramics. A Wheatstone bridge arrangement straddling a bicrystal boundary has been used to verify that spin-dependent electron transfer through a grain boundary is responsible for the low-field magnetoresistance found in polycrystalline samples below T-C. (C) 1999 American Institute of Physics. [S0003-6951(99)00244-2].