Twelve new substituted thiosemicarbazones have been prepared from formylferrocene and 2- and 4-monosubstituted and 4,4-disubstituted thiosemicarbazides. The infrared spectra of these compounds are discussed in some detail. Copper complexes of three of them were synthesized and their structures established. They were found to be strongly paramagnetic. The electronic absorption spectra of the thiosemicarbazones and the copper complexes are reported.