A batch of ZnO thin films, pure and doped with molybdenum (up to 2 mol %), were prepared using the spray pyrolysis technique on glass and silicon substrates. The effect of molybdenum concentration on the morphology, structure and optical properties of the films was investigated. X-ray diffraction (XRD) results show a wurtzite polycrystalline crystal structure. The average crystallite size increases from 30 to 80 nm with increasing molybdenum content. Scanning electron microscopy (SEM) images demonstrate a smooth and homogeneous surface with densely spaced nanocrystalline grains. The number of nuclei increases, growing over the entire surface of the substrate with uniform grains, when the molybdenum concentration is increased to 2 mol %. The estimated root mean square (RMS) roughness values for the undoped and doped with 1 mol % and 2 mol % of ZnO thin films, defined by atomic force microscopy (AFM), are 6.12, 23.54 and 23.83 nm, respectively. The increase in Mo concentration contributes to the increase in film transmittance.