Anion-radical salts (ARS) of TCNQ have been recently in attention focus due to their wide range of possible applications, and due to the discovery of ARS being capable of forming magnetoordered structures. In spite of a long history of TCNQ chemistry, ARS with pyrazine derivative as a cation are not practically known. Pyrazine is the simplest analogue of phenazine (NMP), a constituent of the first organic metal – NMP-TCNQ. ARS TCNQ with N-alkylpyrazinium cations represent a particular interest due to possessing such a nonalkylated nitrogen atom, a cation which may interact quite specifically with TCNQ- anion-radicals or with donor-acceptor interaction of metal cations, that may result in the formation of supramolecular structures. Recently we have reported the first ARS of TCNQ of a quasi-two-dimensional structure (all the previously known ARS of TCNQ are one-dimensional) – (N-Et-Pz)(TCNQ)3. Quasi-twodimensional character of this ARS follows from its structure and the analysis of its electro-physical and optical properties. This salt reveals spin-ladder properties also. Some of the new ARS TCNQ (N-Me-2,5-di-Me-Pz)(TCNQ)2, (N-Et-2,5-di-Me-Pz)(TCNQ)2, (N-Me-2-NH2-Pz)(TCNQ)2, (N-Me-Tetra-Me-Pz)(TCNQ)2, (N-Me-2,6-di-Me-Pz)(TCNQ)2 and (NMeTetra-Py-Pz)TCNQ2 have been synthesized and characterized by XRD, IR-spectroscopy and resistance measurements. For some of these compounds magnetic properties also were measured. Mechanisms where substituents in pyrazine influence on the crystal structures and physical properties of salts were found. Most of the synthesized compounds are quasi-two-dimensional semiconductors. Some of these ARS possess a number of useful properties, such as relatively high electrical conductivity and low melting point. These properties allow to use the ARS in highly efficient electrolytic capacitors and other modern electronic devices.