ABSTRACTWe demonstrate the facile and efficient surface functionalization of vertically-aligned carbon nanotube (VCNT) arrays using an atmospheric pressure plasma jet (APPJ) system. The VCNT arrays were synthesized on Fe-deposited SiO2 wafers using an acetylene carbon source by thermal chemical vapor deposition method. To functionalize the surface of the VCNT arrays, the APPJ system was ignited using nitrogen gas at high voltage of 15 kV and frequency of 25 kHz. We varied the treatment time of the APPJ and the inter-distance between plasma jet and top surface of the VCNT in order to systematically investigate the optimal conditions of the APPJ system. The hydrophobic nature of the as-grown VCNT arrays was drastically changed to hydrophilic character via the facile APPJ treatment. X-ray photoelectron spectroscopy confirmed the formation of hydrophilic functional groups such as hydroxyl and carboxyl groups, and nitrogen-doping-related functionalities such as amines, in addition to pyrrolic- and pyridinic-bonding. The results prove that the APPJ treatment is a facile and efficient method for the surface modification of nanomaterials.