In this study, the morphological and separation characteristics of PVA membranes incorporated with functionalized CNTs are reported. CNTs was extensively characterized using TGA, FESEM, and TEM. The physicochemical properties of PVA-CNTs membranes were characterized using FESEM, tensile test, DSC, and XRD. DSC measurements showed an increase in melting and glass transition temperature, implying enhancement of polymer chains compacting. XRD analysis confirmed the results of DSC and showed that CNTs can promote crystallinity of the PVA membranes. In addition, tensile measurements revealed that incorporating CNTs into the PVA membranes improves their mechanical properties. The synthesized nanocomposite membranes were then evaluated in pervaporation (PV) dehydration of isopropanol (IPA). The separation results showed that incorporating CNTs into the PVA membranes significantly increases water selectivity of the PVA membranes. This can be attributed to the fact that incorporating CNTs compacts and rigidifies PVA matrix and decreases its free volume. Furthermore, permeation of water molecules through the nanocomposite membranes decrease as a result of the polymer chains rigidification. Effects of feed composition and temperature on PVA-CNTs nanocomposite membranes were investigated. Besides, effects of CNTs content on permeation properties and activation energies of PVA membranes were evaluated.