Preparation of beta-eucryptite by the sol-gel process from aluminum nitrate and aluminum-sec-butoxide was investigated. Preparation of beta-eucryptite from aluminum nitrate, TEOS and LiOH resulted to the formation of beta-eucryptite as the major crystalline phase along with a small amount of minor phase(s). Single-phase beta-eucryptite was prepared from aluminum-sec-butoxide, TEOS and LiOEt with the aid of Hacac in 2-methoxyethanol and characterized by XRD and TGA/DSC. The coordination states of aluminum atoms after reaction of aluminum-sec-butoxide with other reactants in the preparation of beta-eucryptite were determined by Al-27 NMR. The Al-27 NMR indicated that before gelation, all aluminum atoms are in the six-coordinated states and infrared (IR) spectroscopy showed that the SiOAl bond forms after gelation which is important for preparation of single-phase beta-eucryptite by the sol-gel method. (C) 2002 Elsevier Science B.V. All rights reserved.