Complexes of Co(II), Mn(II), and Cr(II1) with N-butylurea, N-methylthiourea, and N,N1-dimethylthiourea, and C1-, Br-, NO3-, and C104-anions were prepared and characterized using infrared and visible spectroscopy, and magnetic susceptibility. The urea is bonded through oxygen, and the thioureas through sulfur in all cases. The Co-N-butylurea compounds are octahedral, mostly with CoLGXZ stoichiometries, but some compounds involving coordinated anions and possibly bridging butylurea ligands were found. The Co-thioureas are tetrahedral. Octahedral Cr(II1) con~pounds of the type CrL3X3 and CrLG(C104)3 were prepared, and the CrS, chromophore characterized. Mn(I1)-butylureas arc octahedral, while the thioureas show MnLGXz and MnL4X2 stoichiometries. X-ray diffraction established some of the latter to be isostructural with the analogous tetrahedral Co(I1) compounds. Ligand field parameters Dq and B have been evaluated for the Co(I1) and Cr(II1) con~pounds.