Adsorbent columns, containing different amounts of multi-walled carbon nanotubes (MWCNTs), in a semicontinuous process were studied. The optimal conditions for the discoloration of water contaminated by an azoic organic textile dye were investigated. In particular, as representative of contaminated water, a highly concentrated solution of Reactive Black 5 (RB5) equal to 37 mg/L was utilized. A predetermined volume of dye solution, equal to 100 mL, was subjected to repeated cycles of adsorption until the eluted solution became colorless. This adsorption operation was carried out for different types of columns. Adsorbent performances as a function of characteristics of each column were investigated. For each column, the optimum quantity of MWCNTs, maximum volume of treatable solution, carbon usage rate (CUR), empty bed contact time (EBCT), and adsorption capacity were determined. The permeate was characterized by UV-VIS analysis and TOC analysis, while adsorbent material (MWCNTs) was characterized by thermogravimetric TG-DTA analysis. The column containing 2.5 g of carbon nanotubes was revealed to be the best one for the total amount of Reactive Black 5 adsorbed, i.e., 55 mg/g(MWCNTs) The research has shown the high adsorption efficiency of carbon nanotubes toward RB5 dye, highlighting the degradation of the dye molecule and the stratification, inside the columns, of the adsorbed compound.