A complex study of the adhesion of multi-walled carbon nanotubes to a titanium surface, depending on the modes of irradiation with He + ions of the "MWCNT/Ti" system, was conducted using atomic force microscopy and X-ray photoelectron spectroscopy. A quantitative assessment of the adhesion force at the interface, performed using atomic force microscopy, demonstrated its significant increase as a result of treatment of the "MWCNT/Ti" system with a beam of helium ions. The nature of the chemical bonding between multi-walled carbon nanotubes and the surface of the titanium substrate, which causes this increase in the adhesion of nanotubes to titanium as a result of ion irradiation, was investigated by X-ray photoelectron spectroscopy. It was established that this bonding is the result of the formation of chemical C-O-Ti bonds between titanium and carbon atoms with the participation of oxygen atoms of oxygen-containing functional groups, which are localized on defects in the nanotube walls formed during ion irradiation. It is significant that there are no signs of direct bonding between titanium and carbon atoms.