Thiosemicarbazide derivatives are widely used in medicine to treat different types of diseases. All of them have a wide range of donor atoms to form with metal ions biologically active coordination compounds with various composition and properties. It has been established that in many cases the biological activity of medicaments is consistent with their ability to form complexes. Therefore the synthesis and structure determination of thiosemicarbazide derivatives and its coordination compounds are of both scientific and practical interest. The purpose of this study was to investigate the structural features of salicylaldehyde 4-allylthiosemicarbazone (I), 3-nitro-(II) -, 3-methoxy-(III), 4-hydroxysalicylaldehyde(IV) 4-allylthiosemicarbazones, and their complexes with cobalt (V) and copper (VI, VII) by X-ray metod. The organic compounds I–IV adopt the Z-configuration relatively to the double azomethine bond C=N. These molecules are not planar, the mean square planes of its phenyl cycles are located at angels of 10.7†19.3 to the planar thiosemicarbazide fragments. In V and VI the cobalt and copper atoms coordinate two and one tridentate anionic ligands I respectively which binds to the metals through S, O, N atoms. The cobalt atom forms the octahedral complex, while the Cu(II) ion is in a square planar environment and the fourth coordination site is occupied by the dimethylsulfoxide oxygen atom. In VII the copper atom coordinates tridentate anionic ligand III. The metal has square planar coordination where oxygen atom of water molecule occupies the fourth coordination site.