In this paper, a novel PVA-based polymer nanoparticles/carbon nanotubes (PNP/CNTs) aerogel was successfully developed. Firstly, certain amount water-dispersed carbon nanotubes were introduced into PVA solution and undergo hydrothermal process in the presence of ferric iron to obtain novel PNP/CNTs solution. Then, the PNP/CNTs aerogels were fabricated by the "freeze-thaw" cycle and freeze-drying methods, followed by the vapor deposition of trimethylchlorosilane to obtain hydrophobic aerogel. The morphology and structure of polymer nanoparticles were characterized by SEM, TEM, FT-IR, Raman, UV-vis and XRD. The density, structure and thermal stability of PNP/CNTs aerogel were also investigated. The compressive performance of PNP/CNTs aerogels were better than PVA aerogel and showed small difference before and after hydrophobic treatment. In addition, the adsorption measurements of different aerogels were also studied. The results showed that hydrophobic PNP/CNTs-6 aerogel exhibited better adsorption capacities and reusability than others. These outstanding properties can make PNP/CNTs aerogels considered as a promising candidate to remove organic solvents from aqueous solution. (C) 2020 Elsevier Inc. All rights reserved.