Two π-conjugated oxazoles compounds dissolved in toluene were characterized by the hyper-Rayleigh scattering technique in order to determine the value of the first molecular hyperpolarizability (βHRS). Quantum-chemical calculations using time-dependent density functional theory level were performed to calculate the static and dynamic βHRS theoretical values. Experimental βHRS have shown values of about 42 × 10−30 cm4statvolt−1 and 31 × 10−30 cm4statvolt−1 for both organic compounds, which are in a satisfactory accordance with the calculated results.