The method of preparation of nanostructural materials by means of controlled freeze-drying of a liquid dispersion of nanoparticles or submicron particles, characterized by that the liquid dispersion of nanoparticles or submicron particles is frozen and in this form it is submitted to freeze-drying where the molecules of the dispersion medium are removed at requested rate of sublimation, until their entire disposal by sublimation, while the orientation of the normal vector of the predominant surface of sublimation interface is adjusted as required at arbitrary angle to the vertical line, and the rate of sublimation of frozen material is controlled by the combination of vacuum depth and external heating of sublimation surface of the frozen material.