Palladium(II) complexes of thiones having the general formula [Pd(L) 4 ]Cl 2 , where L = thiourea (Tu), methylthiourea (Metu), N,N 0 -dimethylthiourea (Dmtu), and tetramethylthiourea (Tmtu) were prepared by reacting K 2 [PdCl 4 ] with the corresponding thiones. The complexes have been characterized by elemental analysis, IR and NMR spectroscopy, and two of these, [Pd(Dmtu) 4 ]Cl 2 Á 2H 2 O (1) and [Pd(Tmtu) 4 ]Cl 2 (2), by X-ray crystallography. An upfield shift in the[C=S resonance of thiones in 13 C NMR and downfield shift in N-H resonance in 1 H NMR are consistent in showing sulfur coordination with palladium(II). The crystal structures of the complexes show a square-planar coordination environment around the Pd(II) ions with the average cis and trans S-Pd-S bond angles of 89.64°and 173.48°, respectively.