The present invention relates to layered organic structures in which anisotropic crystalline seed layers control crystalline structure of the subsequent epitaxial organic layers. The structure comprises in sequence a substrate, a globally ordered crystalline seed layer with intermolecular spacing of 3.4.+-.0.3 .ANG., and at least one epitaxial layer of an organic compound. The seed layer is comprised of disc-shaped molecules of at least one polycyclic organic compound with conjugated .pi.-system. At least one layer of an organic compound is epitaxially deposited onto the seed layer. The present invention also provides a method for obtaining a layered organic structure. The method comprises forming of a globally ordered anisotropic crystalline seed layer on a substrate by means of the Cascade Crystallization Process. The seed layer has an intermolecular spacing of 3.4.+-.0.3 .ANG. and it is formed by rodlike supramolecules comprised of disc-shaped molecules of at least one polycyclic organic compound with conjugated .pi.-system. Epitaxially depositing one epitaxial organic layer from the vapor or liquid phase onto the seed layer so as to obtain a layered organic structure.