A facile nonaqueous sol-gel synthesis for Li-Al-O nanoparticles with tunable stoichiometry and phase purity has been developed. Adjusting the reaction conditions, γ-Al 2 O 3 , α-Al 2 O 3 , LiAl 5 O 8 , β-LiAlO 2 , and γ-LiAlO 2 nanoparticles can be synthesized. For the first time, the synthesis of phase-pure nanoscaled β-LiAlO 2 is obtained at low temperature. All the products were characterized by X-ray powder diffraction, Fourier-transformed infrared, small-angle X-ray scattering, transmission electron microscopy/scanning electron microscopy, nitrogen sorption and elemental analysis. The extensive characterization points out some main features for the products: phase purity, nanoscale size, high surface area, good thermal stability, and good dispersion in ethanol. These properties are rarely combined in a single product, making the proposed protocol an important tool for the future applications of Li-Al-O nanoparticles in the field of catalysis and absorptive materials.