The LiTaO3 powders with uniformly sized primary particles have been successfully synthesized using a solid state reaction method. The calcined powders were hot-pressed at 1250°C to form the densest ceramics yet reported of undoped LiTaO3. Neutron and electron backscatter diffraction (EBSD) analysis confirmed a random distribution of grain orientations in the hot-pressed body. Neutron, X-ray, and EBSD studies all indicated the presence of significant residual stresses in the dense ceramic, likely resulting from the large crystallographic anisotropy in thermal expansion of LiTaO3. In addition, EBSD images revealed several unusual microstructural features, presumably related to exaggerated grain growth.