Surface plasmon resonance (SPR) sensing and an enhanced data analysis technique are used to obtain precise predictions of the dielectric constant and thickness of a nanolayer. In the proposed approach, a modified analytical method is used to obtain initial estimates of the dielectric constants and thicknesses of the metal film and a nanolayer on the sensing surface of a SPR sensor. A multiexperiment data analysis approach based on a two-solvent SPR method is then employed to improve the initial estimates by suppressing the noise in the measurement data. The proposed two-stage approach is employed to determine the dielectric constant and thickness of a molecular imprinting polymer nanolayer. It is found that the results are in good agreement with those obtained with an ellipsometer and a high-resolution scanning electron microscope.