Nitrogen is an essential element involved in many interactions in living chemistry, the formation of hydrogen bonds, participation in the acidbase balance in vital systems. It plays a key role in the construction of a huge number of organic and natural compounds. Currently, structural studies of nitrogen-containing compounds require new approaches based on increasingly accurate and proven methods. In this connection, the constants of the spin-spin interaction with 15N nuclei seem to be very promising. In this work, we carried out an extended verification of the 13C15N spinspin coupling constants as a new structural indicator of nitrogen-containing compounds. In this regard, we performed a quantum-chemical calculation of a set of 193 spin-spin coupling values (B3LYP with basis functions 6-311 + + G(2df,2p)) for the set of all currently known conformationally rigid and structurally fixed nitrogen-containing compounds. Comparison of theoretical relationships with experimental ones shows a statistically significant good or excellent agreement. A parallel analysis of the variability of the calculated values of 13C15N spin bonds with the variability of experimental data within groups of related compounds turned out to be practically useful. Such an approach can provide important information for the unambiguous assignment of the 13C peaks and for determining the signs of the 13C15N spinspin coupling constants in cases where they have not previously been established experimentally.