The structural, electronic andmagnetic properties of the three possible terminations of the (001)-oriented thin film of the double perovskite Pb2FeMoO6, 10-L FeMoO4 and PbO terminated, 9-L FeMoO4 terminated and 11-L PbO terminated, have been studied by using the first-principles calculations. It is found that, firstly an outwards relaxation is observed for several layers near surface and the relaxed fractional rumpling s of the PbO layer is larger than that of the adjacent FeMoO4 layer and both have a decrease tend from surface layer to inner layer. Second, whether parallel to or perpendicular to the surface, the Mo-O bond length is always shorter than the adjacent Fe-O bond length. Thirdly, the half-metallic ferromagnetic (HM-FM) character ensures these three terminations of the (001)-oriented thin films of the double perovskite Pb2FeMoO6 a potential application in magnetoresistive and spintronics devices. Fourth, delocalized distribution of the spin charge densities around the Fe atoms on the first FeMoO4 layer leads to a smaller magnetic moment of the Fe atoms on the first FeMoO4 layer than the inner Fe atoms. (C) 2016 Elsevier B.V. All rights reserved.