Surface functionalization of multi-walled carbon nanotubes (MWNTs) was carried out by means of acid treatment. The presence of oxygen functional groups on the surface of acid-treated MWNTs was confirmed with the aid of Fourier transform infrared spectroscopy and X-ray spectroscopy. In addition, carboxylic groups generally formed on the surface of acid-treated MWNTs, and the dispersion was increased by the duration of the acid treatment. The zeta-potential indicated the surface charge transfer and the dispersion of MWMTs. Morphological characteristics of acid-treated MWNTs were also observed using a transmission electron microscopy, X-ray diffraction, and Raman analysis, which was revealed the significantly unchanged morphologies of MWNTs by acid treatment. The hydrogen adsorption capacity of the MWNTs was evaluated by means of adsorption isotherms at 77 K/1 atm. The hydrogen storage capacity was dependent upon the acid treatment conditions and the formation of oxygen functional groups on the MWNT surfaces. The latter have an important effect on the hydrogen storage capacity.