Vertically aligned multiwalled carbon nanotubes (v-CNTs) were functionalized with oxygen groups using low kinetic energy oxygen ion irradiation. X-ray photoelectron spectroscopy (XPS) analysis indicates that oxygen ion irradiation produces three different types of oxygen functional groups at the CNTs surface: epoxide, carbonyl and carboxyl groups. The relative concentration of these groups depends on the parameters used for oxygen ion irradiation. Scanning electron microscopy (SEM) shows that the macroscopic structure and alignment of v-CNTS are not affected by the ion irradiation and transmission electron microscopy (TEM) proves tip functionalization of v-CNTs. We observed that in comparison to oxygen plasma treatment, oxygen ion irradiation shows higher functionalization efficiency and versatility. Ion irradiation leads to higher amount of oxygen grafting at the v-CNTs surface, besides different functional groups and their relative concentration can be tuned varying the irradiation parameters.