Catalyst-free chemical vapor deposition is used to form thin (1-2 nm) carbon layers on the surface of alumina nanofibers resulting in carbon-alumina nanocomposites. Thermal analysis, X-ray fluorescent microanalysis, Raman spectroscopy, and electrical resistance measurements of these composites show that increasing of synthesis time not only increases the amount of carbon on alumina surface, but also the ordering and density of the carbon layers. Nitrogen adsorption data reveal the decrease of total pore volume with increasing the synthesis time. The obtained composite material could be employed for the preparation of ion-selective membranes with switchable ion transport, electroconductive ceramics, and electrochemical sensors.