Nanocrystalline sodalite has been synthesized by a non-hydrothermal route from a solid gel mixture of Al2O3 pillared clay and NaOH at 80 °C. The nucleation and crystal growth mechanism for the solid−solid transformation were studied using X-ray diffraction (XRD), 27Al and 29Si MAS NMR, SEM, and HRTEM. Compared with hydrothermal synthesis of zeolites, the microporous Al2O3 pillared clay is rapidly transformed into three-dimensional zeolitic sodalite without undergoing a noticeable X-ray amorphous phase. Likewise, 27Al and 29Si NMR obviously reveal that the local environments around Al and Si rapidly evolve into a zeolitc Al−O−Si framework at the initial stage of reaction. Scanning electron micrographs indicate that the resulting products are composed of nanometer-sized sodalite particles (ca. 30−50 nm) with the lamellar character of pristine layered clay. HRTEM images clearly demonstrate both formations of sodalite nuclei through localized solid−solid transformation of an aluminosilicate matrix and crystal...