The book is devoted to the consideration of the different processes taking place in the films and at surfaces. Where it is possible, these processes are considered in the frame of the unified theoretical approach. Since the most important physico-chemical phenomena in such media are accompanied by the rearrangement of an intra- and intermolecular coordinates and consequently a surrounding molecular ensemble, the theory of radiationless multi-vibrational transitions is used for its description. So the first part of the monograph includes: The second part of the book considers the numerous surface phenomena (formation of point defects, spectral characteristics, diffusion, phase transitions and catalytic reactions). And in the third part is described the preparation methods and characteristics of different types of thin films (chemical vapor deposition, Langmuir-Blodgett, sol-gel, vacuum magnetron sputtering, laser electrodispersion) as well as processes proceeding in them (growth mechanisms, chemical reactions spectral characteristics, and thermodynamic, optical, electrical, magnetic, transport and sensor properties). The description of all these observed phenomena is conducted based on the theoretical approaches considered in the first part of the book. Both experimental and theoretical descriptions are represented. Media rearrangement coupled with the reagent transformation largely determines the absolute value and temperature dependence of the rate constants and other characteristics of the considered processes. These effects are described at the atomic or molecular level based on the multi-phonon theory, starting from the first pioneering studies through to contemporary studies. A number of questions are included at the end of many chapters to further reinforce the material presented.