Vanadium salts and well-known vanadium coordination compounds have shown antibacterial, antifungal, antitumor, and antidiabetic activities when investigated by various biological methods [1,2]. Our goal was, firstly, to synthesize and characterize two enantiomers of a vanadium complex with Schiff-base ligandderived from salicylaldehyde and valine and, secondly, to evaluate their antitumor properties. Condensation of 2-hydroxybenzaldehyde (salicylaldehyde, sal) with L-valineor D-valine (L/D-val), respectively, yielded the tetradentate Schiff bases: H2(sal-L-val) and H2(sal-D-val). Dinuclearoxovanadium(V) complexes with the molecular formulas: [(VO)2(m2-O)(sal-Lval) 2(H2O)] (L-CP) [3] and [(VO)2(m2-O)(sal-D-val)2(H2O)] (D-CP) have been synthesized and characterized. Bothcomplexes have been characterized by elemental analysis, single-crystal X-ray diffraction, X-ray powder diffraction, and spectroscopic (IR, UV-Vis and circular dichroism) measurements.The protein binding capacity of the compounds was tested in vitro by a fluorometric method based on quenching the fluorescence of bovine serum albumin (BSA). Cytotoxic effects of compounds were examined on hepatocyte carcinoma (HepG2) cell line using XTT assay. The spectral and structural data revealed that the coordination of tridentate/tetradentate L/D-Schiff base ligands to vanadium atoms lead to binuclear complexes in which V (V) atoms have distorted octahedral coordination geometry and the compounds exhibit optical activity. The compounds bind and quench the intrinsic fluorescence of BSA in a dose-dependent manner. They do not show cytotoxic effects on HepG2 cells at concentrations below 100 μM, but induce approximately 70% for L-CP and 60% for D-CP cell death at a concentration of 300 μM. We have synthesized and physicochemical characterized two binuclear vanadium complexes derived from salicylaldehyde and L-valine and D-valine, respectively. Moreover, owing totheir capacity to bind to BSA and to induce cell death against HepG2 cells, the synthesized compoundsmay be the ideal candidates for cancer therapy.