AbstractAmorphous, as shown by X‐ray diffraction measurements, MoS2 films (a‐MoS2) were deposited by heating a molybdenum wire at temperatures between 500 and 700 °C in H2S at 1 Torr. As shown by Scanning Electron Microscopy measurements, the morphology of samples depends significantly on the filament temperature; at low temperature samples are homogeneous and smooth, at intermediate temperatures they exhibit a granular microstructure and at high temperatures a columnar one. X‐ray photoelectron spectroscopy measurements have shown S/Mo ratios in films varying between 2.5 and 1.5 dependent on filament temperature. Films also contain oxygen at atomic contents of 8 to 12%. As shown by XPS and Raman spectroscopy, at a filament temperature of 600 °C films are mainly composed of MoS2 also containing oxygen at an atomic ratio of 8%. Spectroscopic ellipsometry measurements made on a‐MoS2 films have shown that their band gap is of the order of 1.4 eV, slightly higher than that for the bulk crystalline material. Photoluminescence spectroscopy measurements have shown that samples exhibit a doublet of peaks at 2.8 and 3 eV blue shifted relatively to MoS2 samples composed of one or two mono‐layers. The above indicate that the electronic structure of crystalline atomic‐layer thick MoS2 is preserved in a‐MoS2 films. (© 2015 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)