Single-crystalline thin films of Sr2MoO4 with K2NiF4 structure have been epitaxially grown by a pulsed laser deposition on SrTiO3(1 0 0) and DyScO3(1 1 0) substrates. Phase-pure and high crystalline quality films were obtained in quite a narrow window of growth condition. The resistivity shows a metallic behavior and the residual resistivity is about two orders of magnitude lower than that of polycrystalline samples. Such single-crystalline Sr2MoO4 films are suitable for examining the physical properties and exploring heterostructures with other oxides. (C) 2011 Elsevier B.V. All rights reserved.