This work focused on the facile synthesis of carbon nanotubes grafted with a polymer of trimesoyl chloride and m-phenylenediamine (CNTs-MDP-TMC) as novel and effective adsorbent and investigation of its ability in the phenol uptake from aqueous media. The chemical and morphological characterization of the synthesized adsorbent was carried out by FT-IR, SEM, EDX, and mapping techniques. The influence of the operational parameters on the adsorption performance was inspected and optimized batch adsorption conditions by factorial design analysis. The non-linear Langmuir model was better represented the isotherm of phenol adsorption compared to the Freundlich isotherm. The CNTs-MDP-TMC had a maximum adsorption capacity as much as 261.6 mg/g. The kinetic examinations revealed that the pseudo-second-order (PSO) kinetic model depicted higher relationship with phenol adsorption than the pseudo-first-order (PFO) model. The thermodynamics findings confirmed that the phenol adsorption by the CNTs-MDP-TMC is taken place exothermically and more spontaneously with lessening temperature. The prepared adsorbent had a great adsorption/desorption performance, especially during the first four cycles. It can be drawn a conclusion form all findings that the synthesized CNTs-MDP-TMC has great prospective as a novel and influential adsorbent for phenol polluted-wastewaters.