Palladium(II) and platinum(II) complexes of N-ethyl-N′-pyrimidin-2-ylthiourea(HL1) and N-phenyl-N′-pyrimidin-2-ylthiourea (HL2) have been prepared, and the complexes [M(HL)Cl2], [Pt(L)2], [Pd(HL1)2]Cl2, and [Pd(L2)2] (where M = PdII or PtII) were characterized. The spectroscopic data are consistent with coordination of thioureas as neutral or monoanionic ligands to PdII and PtII through S and a pyrimidine-N. The IR spectra show shifts of CS and pyrimidine ring stretch bands to lower and higher frequencies, respectively. The 1H NMR spectra differentiate between H(4′) and H(6′) resonances and indicate downfield shifts for all protons of pyrimidine [H(4′), H(5′), and H(6′)], two resonances for two N‒H protons for complexes containing the neutral ligand (HL), and only one N‒H proton chemical shift for complexes containing the monoanion (L). 13C NMR chemical shifts of pyrimidine carbons are correlated with the type of bonding between PdII or PtII and pyrimidine-N. The magnetic susceptibilities suggest a diamagnetic planar structure for all complexes. Supplemental materials are available for this article. Go to the publisher's online edition of Phosphorus, Sulfur, and Silicon and the Related Elements to view the free supplemental file.