Two series of copper(II) complexes with thiosemicarbazide (Tsc) have been prepared, and their ultraviolet and visible reflectance spectra, infrared spectra, and magnetic properties have been measured and are discussed. The L1 series of the type CuTscX2(X = Cl, Br, or ½SO4) is thought to have a polymeric structure. Complexes in the L2 series, CuTsc2X2(X = Cl, Br, No3, ClO4, or ½SO4), have distorted octahedral structures.