The effect of O2+, H2++ O2+, and N2++ O2+ ion-beam irradiation of carbon nanotubes (CNTs) films on the chemical and electronic properties of the material is reported. The CNTs were grown by the chemical vapor deposition technique (CVD) on silicon TiN coated substrates previously decorated with Ni particles. The Ni decoration and TiN coating were successively deposited by ion-beam assisted deposition (IBAD) and afterwards the nanotubes were grown. The whole deposition procedure was performed in situ as well as the study of the effect of ion-beam irradiation on the CNTs by x-ray photoelectron spectroscopy (XPS). Raman scattering, field-effect emission gun scanning electron microscopy (FEG-SEM), and field emission (FE) measurements were performed ex situ. The experimental data show that: (a) the presence of either H2+ or N2+ ions in the irradiation beam determines the oxygen concentration remaining in the samples as well as the studied structural characteristics; (b) due to the experimental conditions used in the study, no morphological changes have been observed after irradiation of the CNTs; (c) the FE experiments indicate that the electron emission from the CNTs follows the Fowler-Nordheim model, and it is dependent on the oxygen concentration remaining in the samples; and (d) in association with FE results, the XPS data suggest that the formation of terminal quinone groups decreases the CNTs work function of the material.