A platelike mesocrystalline BaTiO3/SrTiO3 (BT/ST) nanocomposite is prepared via a clever two-step solvothermal soft chemical process. First a protonated titanate H1.07Ti1.73O4路nH2O (HT) crystal with a layered structure and platelike morphology is solvothermally treated in a Ba(OH)2 solution to generate a homogeneous platelike BaTiO3/HT (BT/HT) nanocomposite. Second the generated BT/HT nanocomposite is solvothermally treated in a Sr(OH)2 solution to generate the mesocrystalline BT/ST nanocomposite with platelike particle morphology. The transformation reactions from the HT precursor to the mesocrystalline BT/ST nanocomposite are topochemical conversion reactions, and the formed BT/ST nanocomposite is constructed from well-aligned BT and ST nanocrystals in the same crystal-axis orientation. The BT/ST nanocomposite annealed at 900 掳C shows a ferroelectric behavior and drastically enhanced piezoelectric and dielectric responses owing to the introduction of a lattice strain at a three-dimensional heteroepitaxial interface between the BT and ST nanocrystals in the mesocrystal. The nanostructure of the BT/ST mesocrystal is suitable for simultaneous application of the strain engineering and the orientation engineering to develop high performance piezoelectric and dielectric materials.