Three copper systems with relevance to materials technology are discussed. In the first, a CuS precursor, Cu4S 10(4-methylpyridine)4 (4-MePy), was prepared by three routes: reaction of Cu2S, reaction of CuBr•SMe2 and oxidation of copper powder with excess sulfur in 4-methylpyridine by sulfur. In the second, copper powder was found to react with excess thiourea (H2NC(S)NH2) in 4-methylpyridine to produce thiocyanate (NCS-) complexes. Three isolated and characterized compounds are: Cu(NCS)(4-MePy)2, a polymer, [4-MePy•H][Cu(NCS)3(4-MePy)2], a salt, and t-Cu(NCS)2(4-MePy)4. Finally, an attempt to produce a mixed-metal sulfide precursor of Cu and Ga in N-methylimidazole (N-MeIm) resulted in the synthesis of a Cu-containing polymer, Cu(S04)(N-Melm). The structures are presented; the chemistry will be briefly discussed in the context of preparation and processing of copper-containing materials for aerospace applications.