Nanocrystalline zeolites are emerging as important materials for a variety of potential applications in industry and medicine. Reducing the particle size to less than 100 nm results in advantages for nanocrstalline zeolites relative to micrometer-sized zeolite crystals, such as very large total and external specific surface areas and reduced diffusion path lengths. Understanding the physical and chemical properties of zeolite nanocrystals is imperative for further development and application of nanocrystalline zeolites. In this study, the framework stability of nanocrystalline NaY zeolite with a crystal size of 66 nm and Si/Al = 1.74 was investigated at pH 7.4, 4, 2, and 1. The solids and solutions were analyzed using several different analytical techniques. The relative crystallinity and crystal size and morphology of the solids were examined by powder X-ray diffraction (MUD) and transmission electron microscopy (TEM), respectively. The aluminum content, Si/Al, and coordination were monitored by inductively coupled plasma/optical emission spectroscopy (ICP/OES), X-ray photoelectron spectroscopy (XI'S), and aluminum-27 solid-state magic-angle spinning NMR. As the acidity of the medium increased, the framework stability of nanocrystalline NaY decreased. Treatment of the zeolite samples at pH 1 resulted in complete degradation of the zeolite framework after 1 h. An increase in Si/Al was also observed, suggesting the selective removal of aluminum at low pH.