This chapter presents the possibility of forming nanocrystalline structure and design properties of materials by electrocrystallization method. The basis of the electrocrystallization process and factors determining the result of the processes under considerations are presented. The electrocrystallization method was used for producing metal materials Cu and Ni and nanocrystalline structure of the nanocrystalline composite materials with matrix Cu, Ni, and nanosized particles of the disperse phase in the form of Al 2 O 3 , Si 3 N 4 , and CNTs. Methods of X-ray diffraction (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM) were applied for the complete characterizations of the dispersion phases and the structure of the produced materials. The results of these studies are presented in the form of the corresponding images and graphs.