New 3-aryl(hetaryl)-1-(benzo[d]thiazol-2-yl)-6-methyl-5-phenylverdazyls were synthesized and characterized by EPR and IR spectroscopies, mass spectrometry, cyclic voltammetry, and X-ray diffraction. The effect of substituents on the spectral and electrochemical properties was studied. It was shown that substituents at position 3 of the verd azyl tetrazine ring, regardless of their nature, cause a significant shift of the oxidation and reduction potentials to the anodic region. The results obtained suggest that the synthesized compounds can be used as an electroactive components in rechargeable organic batteries.