Carboxylated multi-walled carbon nanotubes (MWNTs) were in detail characterized by XRD, XPS, FTIR, and thermogravimetric measurements. Carboxylic acid groups were functionalized to MWNTs under aqueous acid condition. The changes of sonication and reflux conditions rarely influenced the degree of carboxylation on MWNTs, but decreased the thermal stability of the resultant carboxylated MWNTs. XRD results showed that the diffraction peaks (100), (101), and (102) of pristine MWNTs disappeared after acid treatment, but the diffraction peak (002) was Preserved in the carboxylated MWNTs. The introduction of carboxylic acid groups on MWNTs caused to improve the dispersibility of the resultant carboxylated MWNTs in water.