Liquid ammonia was used to treat films of nanofibrillated cellulose (NFC), trimethylammonium-modified NFC (TMA-NFC), and their composites with vermiculite. Crystal structure, mechanical properties, water vapor permeation and water vapor adsorption of the resulting materials were investigated. Upon treatment, the crystal structure of (TMA-)NFC both in presence and absence of vermiculite changed from cellulose I to III. With the exception of TMA-NFC/vermiculite composites, pronounced effects on the addressed mechanical properties arose after exposure of the materials to ammonia. Furthermore, treatment of composite films with ammonia led to a distinct decrease in water vapor permeation. Remarkably, TMA-NFC/vermiculite composites films show the best water vapor barrier properties, high-