The micro- and nanoscale morphologies of thin nanocomposite films comprising an immiscible nylon 6/polyethylene blend reinforced with modified sodium montmorillonite were found to substantially affect water vapor transmission rates (WVTRs). Maleic anhydride-grafted high-density polyethylene was incorporated as a compatibilizer between the nylon and polyethylene phases. Preferential incorporation of an organosilicate nanoclay in the nylon phase had a secondary effect on the overall blend morphology and thermal properties. Different degrees of phase continuity in the nanocomposite blend system were studied for their effect on WVTRs by varying the relative viscosities of the polymer phases. Transmission electron and atomic force microscopy were utilized to reveal the morphologies of the nanocomposite blends. POLYM. ENG. SCI., 54:1341-1349, 2014. (c) 2013 Society of Plastics Engineers