In this work, the refractometry method was used to study of the molecular interactions and structural characteristics of dimethylformamide-ethanol and cyclohexane-ethanol binary mixtures. The refractive indices of mixtures were measured over a wide range of dimethylformamide and cyclohexane concentrations (0−1.0 mole fractions) at 25°С. It has been shown that heteromolecular complexes in binary solutions are formed at the concentration of ∼0.5 mole fraction of those compounds due to strong H-bonds. Relatively weak interactions are determined at a concentration of ∼0.2 and ∼0.9 mole fraction of dimethylformamide and ∼0.2 and ∼0.8 mole fraction of cyclohexane.