Thiosemicarbazide derivatives are widely used in medicine in treating various types of diseases. All of them have a wide range of reactive atoms and form with metal ions coordination compounds with various composition, structure, and properties. Many of these coordination compounds are biologically active substances. Therefore, they can be used as base materials for creating new antimicrobial, antitumor, antifungal, and antituberculous drugs, as well as for selective microbiologic nutritional media, disinfectants, antiseptics. Therefore, the synthesis and study of new coordination compounds of biometals with thiosemicarbazones is both of scientific and practical interest. The aim of this work is finding the optimal conditions of synthesis, determination of the composition, structure, physicochemical, antimicrobial, and antitumor properties of the coordination compounds of chromium, manganese, iron, cobalt, nickel, copper, and zinc with 4allylthiosemicarbazones (H2L1-9) of salicylaldehyde (H2L1), 3-hydroxy-(H2L2), 3-methoxy-(H2L3), 3-nitro-(H2L4), 4-hydroxy-(H2L5), 5-bromo-(H2L6), 5-nitro-(H2L7), 5hydroxy-(H2L8), and 3,5-dibromosalicylaldehydes (H2L9). N OH NH S R3 R2 R1 H2L1-9 = NH H2L1 : R1 =R2 = R3 = H; H2L2 : R1 = R2 = H, R3 = OH; H2L3 : R1 = R2 = H, R3 = CH3O; H2L4 : R1 = R2 = H, R3 = NO2; H2L5 : R1 = R3 = H, R3 = OH; H2L6 : R1 = Br, R2 = R3 = H; H2L7 : R1 = NO2, R2 = R3 = H; H2L8 : R1 = OH, R2 = R3 = H; H2L9 : R1 = R3 = Br, R2 = H. The stated above thiosemicarbazones (H2L1-9) have been synthesized by condensation of 4-allylthiosemicarbazide with respective aldehyde in 1:1 molar ratio. Their purity was proved by NMR spectroscopy (1H, 13C, and 15N). The structures of H2L1, H2L3, H2L4, and H2L6 were proved by X-ray diffraction analysis. The composition and structure of the synthesized coordination compounds were determined on the basis of data from IR spectroscopy, magnetochemical research, and X-ray diffraction analysis. Synthesized coordination compounds show selective antimicrobial activity towards a series of standard strains Staphylococcus aureus (ATCC 25923), Enterococcus faecalis, Escherihia coli (ATCC 25922), Salmonella abony (GISK 03/03), and Candida albicans in the range of concentration 0.0015-0.5 mg/mL. Moreover, the sinthisezed coordination compounds inhibit the human promyelocytic leukemia HL-60 cells’ proliferation up to 100% in the range of concentration 10-5 -10-6 mol/l.