Uniform carbon nanofiber films and nanofiber composite coatings were synthesized from ethylene on nickel coated alumina substrates by laser-assisted catalytic chemical vapor deposition. Laser annealing of a 50 nm thick nickel film produced the catalytic nanoparticles. Thermal decomposition of ethylene over nickel nanoparticles was initiated and maintained by an argon ion laser operated at 488 nm. The films were examined by scanning electron microscopy and by transmission electron microscopy. Overall film uniformity and structure were assessed using micro-Raman spectroscopy. Film quality was related to the experimental parameters such as incident laser power density and irradiation time. For long irradiation times, carbon can be deposited by a thermal process rather than by a catalytic reaction directly over the nanofiber films to form carbon nanocomposite coatings. The process parameters leading to high quality nanofiber films free of amorphous carbon by-products as well as those leading to nanofiber composite coatings are presented. (c) 2006 Elsevier B.V. All rights reserved.