Barium titanate (BaTiO3, BT) and strontium titanate (SrTiO3, ST) nanocube particles were prepared by a solvothermal method. The prepared particles were collected by a centrifugal separator. The X-ray diffraction (XRD) measurement and a transmittance electron microscope (TEM) observation confirmed the formation of perovskite BT and ST nanocube particles with sizes of around 17 nm. These nanocube particles were monodistributed in hexane with tri-n-butylphosphine oxide (TBPO) as dispersant, separately, and then, the accumulations composed of the BT and ST nanocubes were built up using a selective catalytic reaction between 3-bromopropylphosphonic acid (BP) and aminomethylphosphonic acid (AM) as smart glue. The TEM observation confirmed that a part of accumulations showed a hetrointerface connection between BT and ST.