A novel two-step process has been developed for the preparation of Ba(0.9)Ca(0.1)TiO(3) plate-like grains with [110]-crystal-axis-orientation. In the first step, plate-like particles of a layered titanate H(1.07)Ti(1.73)O(4) are solvothermally treated in a Ba (OH)(2)-Ca(OH)(2) mixed solution, and then in the second step, heat-treat the solvothermally treated sample to complete the formation reaction of Ba(0.9)Ca(0.1)TiO(3). The formation reaction and nanostructure of the Ba(0.9)Ca(0.1)TiO(3) plate-like grains were characterized using X-ray diffraction, FE-SEM, TEM, and SEAD. The Ba(0.9)Ca(0.1)TiO(3) plate-like grains are constructed from spherical nanoparticles with particle size of about 10-20 nm. The spherical nanocrystals in each plate-like grain arrange in the same crystal-axis-orientation direction, which presented a diffraction pattern similar to the single crystal. The Ba(0.9)Ca(0.1)TiO(3) plate-like grains were utilized to fabricate an oriented Ba(0.9)Ca(0.1)TiO(3) ceramic to demonstrate the potential application of the plate-like grains, and the [110]-oriented Ba(0.9)Ca(0.1)TiO(3) ceramic with a high degree orientation of F(110) = 76% and small grain size of about 1-2 mu m was obtained.