This study aimed to describe the adsorption process of ortho-dichlorobenzene (o-DCB) onto activated carbons (ACs) and modified carbon nanotubes (CNTs) from the aqueous phase. The starting material NC_7000 carbon nanotubes were modified by chlorination (NC_C) and then by the introduction of hydroxyl groups (NC_C_B). The concentration of o-DCB in solutions was performed by UV-VIS spectrophotometry. After adsorption, the activated carbons were regenerated by extraction with organic solvents such as acetone, methanol, ethanol, and 1-propanol; the carbon nanotubes were regenerated by methanol. The degree of adsorbate recovery was determined by gas chromatography (GC) with flame ionization detection, using ethylbenzene as an internal standard. The equilibrium isotherm data of adsorption were satisfactorily fitted by the Langmuir equations. The results indicate that carbon adsorbents are effective porous materials for removing o-DCB from the aqueous phase. Additionally, activated carbons are more regenerative adsorbents than carbon nanotubes. The recoveries of o-DCB from ACs were in the range of 76–85%, whereas the recoveries from CNTs were in the range of 23–46%. Modifications of CNTs affect the improvement of their adsorption properties towards o-DCB compared to unmodified CNTs. However, the introduction of new functional groups on carbon nanotube surfaces makes the regeneration process less effective.