© 2015 Pleiades Publishing, Ltd. The structures of complexes [Pt(Bt)(μ-(N^S))]2 with platinated 2-phenylbenzothiazole (Bt) and bridging 2-mercapto derivatives (NS) of thiazoline, 1-methylimidazole, and pyrimidine in the crystalline state and in a CDCl3 solution are studied by X-ray diffraction analysis and 1H, 13C, and 195Pt NMR spectroscopy. Complexes [Pt(Bt)(μ-(N^S))]2 have the cis-N(Bt),S(N^S) structure with the Pt-Pt chemical bond (2.89-2.93 Å) and antisymmetrical position of two cycloplatinated and two bridging ligands (CCDC nos. 1001204 (I), 1027021 (II), and 993566 (III)). The long-wavelength absorption bands (410-540 nm), phosphorescence bands with λmax = 685 nm, and two-electron electroreduction (E p = -(2.00-2.27) V) and oxidation (E p = 0.07-0.20 V) processes are assigned to photo- and electrostimulated processes involving the LUMO and HOMO predominantly localized on the πorbitals of {Pt(Bt)} and on t