Fine beta-Li2TiO3 particles were synthesized by hydrothermal reaction. Lithium vacancies and titanium substitution existed in the (002) lattice plane (pure lithium layer) via hydrothermal reaction, while after calcination, the titanium ions diffuse away from the (002) lattice plane into the LiTi2 layer, confirmed by two-dimensional fast Fourier transformation spectrum of the high-resolution transmission images and the Raman spectra.