We report on the preparation and characterization of epitaxial thin films of the double-perovskite Sr2CrWO6 by pulsed laser deposition. On substrates with low lattice mismatch like SrTiO3, epitaxial Sr2CrWO6 films with high crystalline quality can be grown in a molecular layer-by-layer growth mode. Due to the similar ionic radii of Cr and W, these elements show no sublattice order. Nevertheless, the measured Curie temperature is well above 400 K. Due to the reducing growth atmosphere required for double perovskites, the SrTiO3 substrate surface undergoes an insulator–metal transition impeding the separation of thin film and substrate electric transport properties. © 2003 American Institute of Physics.