The present study describes a novel preparative route to sodalite from layered aluminosilicates such as kaolinite, montmorillonite, and Al2O3-pillared montmorillonite (Al-PILC), those which are subjected to react directly with sodium hydroxide as low as 100 degreesC under an ambient atmosphere. Powder X-ray diffraction (XRD) analysis, infrared absorption (IR) spectra and Al-27 and Si-29 magic-angle-spinning nuclear magnetic resonance (MAS NMR) spectra reveal that the resulting solid products are crystalline sodalites with cubic symmetry (a= 8.92 +/- 0.05 Angstrom) consisted of zeolitic Al-O-Si networks with an alternating ordering of Al and Si tetrahedra. Scanning electron microscopy (SEM) indicates that the sodalites derived from the two-dimensional alummosilicates consist of nano-sized sodalite particles (30-50 nm) with preserved lamellar characters of the pristine layer silicates. Among the starting aluminosilicates, Al2O3-pillared montmorillonite is found to be an active precursor to zeolitic sodalite because of the high microporosity and the compositional and structural similarities.