This paper deals with the synthesis, characterization, and studies of biological properties of a series of 5 coordination compounds based on binuclear core [Mo^(V)₂O₂S₂]²⁺ with thiosemicarbazones ligands bearing different substituents on the R¹ position of the ligand. The complexes are first studied using MALDI-TOF mass spectrometry and NMR spectroscopy to determine their structures in solution in relation to single-crystal X-Ray diffraction data. In a second part, the antifungal and antioxidative activities are explored and the high potential of these coordination compounds compared to the uncoordinated ligands is demonstrated for these properties. Finally, DFT calculation provides important support to the solution studies by identifying the most stable isomers in each [Mo₂O₂S₂]²⁺/Ligand system, while the determination of HUMO and LUMO levels is performed to explain the antioxidative properties of these systems.