The monograph covers theoretical aspects of the method based on the analysis of NMR spectra transformed by electron-nuclear or hyperfine coupling, and provides examples of its practical application for the solution of different tasks related to structure and intramolecular dynamics of multi-electron systems. The fundamentals of NMR theory in paramagnetic systems were formulated by Blombergen, Mc Connell, Solomon, Berkheyn and other researchers. However, wide application of HFC specifics for the solution of diverse chemical tasks was triggered later, after the development of a method for analysis of NMR spectra transformed by additives of paramagnetic complexes. The book consists of three chapters. Chapter 1 discloses the fundamentals of high resolution NMR spectra transformed by hyperfine coupling. The two other chapters illustrate fruitfulness and prospects of the application of NMR phenomenon in paramagnetic systems for studying molecular structure. Examples of specific spectra, analyzed in the monograph, are selected in such a way that they could help a reader understand a circle of possible problems which are solved using peculiarities of the NMR phenomenon in paramagnetic systems. The same examples also illustrate the techniques which can be employed for obtaining information on the molecular structure of both ligands and complexes using their NMR spectra transformed by hyperfine coupling.