New ethynyl derivatives were synthesized from 5-(benzothiazol-2-yl)-1-(4-iodophenyl)-3-phenyl-6-vinyl(phenyl)verdazyls using Sonogashira cross-coupling reactions carried out in two stages. The resulted radicals were characterized using EPR, IR, UV/Vis spectroscopy, mass spectrometry, and cyclic voltammetry. Electronic structure calculations using quantum chemistry methods were performed to analyze some experimental results.