Pulsed Laser Deposition has been used to synthesize Ba(Co,Zn)(1/3)Nb2/3O3 (BCZN) dielectric thin films on MgO (001) substrates. The BCZN films are epitaxial and have an orientation of (001) // MgO (001) and (100) // MgO (100) when deposited at substrate temperatures above 500 degrees C. The film grown at 800 degrees C has the best structural quality, with an X-ray diffraction rocking curve width of similar to 0.5 degrees and a channeling Rutherford Backscattering Spectrometry chi(min) value of 8.8%. The surface roughness decreases monotonically with increasing substrate temperature, with a similar to 3 nm root mean square roughness value for the films deposited at 700 degrees C. Optical transmission measurements indicate a strong direct transition at similar to 4 eV and a refractive index of 2.0 in the visible range. A low-frequency dielectric constant of 34 was measured using a planar interdigital contact structure. The resistivity of the film is 3x10 (10) Omega cm at room temperature and has a thermal activation energy of 0.66 eV. (C) 2013 Elsevier B.V. All rights reserved.