Thin films and coatings are a basis for many technological processes, including microelectronics, electrochemistry and catalysis. The successful deposition of metal films and nanoparticles by chemical vapour deposition (CVD) needs control over a number of physico-chemical processes such as precursor and substrate selection, delivery, temperature, pressure and flow conditions. Here, cobalt thin films were deposited by means of pulsed-spray evaporation chemical vapour deposition (PSE-CVD) from ethanol solutions of Co(acac) 2 and Co(acac) 3 on bare glass and silicon substrates. The physico-chemical properties of the grown films were characterised by XRD (X-ray diffraction), XPS (X-ray photoelectron spectroscopy) and HIM (helium ion microscopy). Co(acac) 2 enabled the growth of cobalt metal at lower temperatures than Co(acac) 3 . The difference in deposition Brought to you by | University of Windsor Authenticated Download Date | 9/29/15 1:02 AM 2 | K. Kohse-Höinghaus et al. temperature was attributed to the ability of ethanol to reduce Co(acac) 2 better than Co(acac) 3 . In addition, the film deposited from Co(acac) 2 exhibited a higher metal content and a less porous structure than that deposited from Co(acac) 3 . Increasing the substrate temperature enhanced the carbon content because of the thermal decomposition of both precursors. Using a nickel seed layer improved the growth rate until a critical temperature of 360 ∘ C, at which the thermal decomposition of the precursor becomes predominant. A decrease in the deposition temperature when using the nickel seed layer was only observed with Co(acac) 2 precursor; the growth behaviour under these conditions was monitored with a unique UHV-compatible PSE-CVD reactor directly attached to an XPS system and ascribed to an enhancement of its catalytic reduction by ethanol.