The results of studies in the field of interfacial synthesis and interfacial formations in liquid–liquid systems are summarized. The mechanisms of the processes of interfacial synthesis are considered. Data on the self-assembly of nanoparticles, films, and 3D materials are given. The properties of materials of interfacial formations in systems with rare-earth elements and di(2-ethylhexyl)phosphoric acid, obtained both in the presence and absence of local vibrations, are described. It was established that materials obtained in the presence of local vibrations in the interfacial layer have higher density, melting point, and magnetic susceptibility and lower electric conductivity. The effect of force field parameters on the properties of interfacial formations is considered. Practical applications and prospects for research in the field of interfacial formations are discussed.