An ethanol gas sensor based on carbon nanofibers (CNFs) with various densities and nanoparticle functionalization was investigated. The CNFs were grown by means of a Plasma-Enhanced Chemical Vapor Deposition (PECVD), and the synthesis conditions were varied to obtain different number of fibers per unit area. The devices with a larger density of CNFs lead to higher responses, with a maximal responsivity of 10%. Furthermore, to simultaneously improve the sensitivity and selectivity, CNFs were decorated with gold nanoparticles by an impaction printing method. After metal decoration, the devices showed a response 300% higher than pristine devices toward 5 ppm of ethanol gas. The morphology and structure of the different samples deposited on a silicon substrate were characterized by TEM, EDX, SEM, and Raman spectroscopy, and the results confirmed the presence of CNF decorated with gold. The influence of operating temperature (OT) and humidity were studied on the sensing devices. In the case of decorated samples with a high density of nanofibers, a less-strong cross-sensitivity was observed toward a variation in humidity and temperature.