Compact cross-flow micro-nebulizer system was developed to introduce the liquid raw materials into the atmospheric-pressure microplasma deposition system, which can control the feed rate of liquid sample to be less than 30 mu l/min. As the first study of the injection of liquid raw material, ethanol or ferrocene/ethanol solution was introduced through the developed nebulizer system to deposit nano-carbon materials, and carbon nanoonions (CNOs) and carbon nanotubes (CNTs) were deposited selectively on the localized area of the glass-epoxy substrate kept toward the downstream of the microplasma jet. The reaction processes during the deposition were discussed based on the optical emission spectroscopy, which strongly indicates the role of OH radicals from the decomposition of ethanol for the selective formations of the CNO and CNTs.