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In this paper, the dynamics of polymer surface and its interior are measured by using fluorescence correlation spectroscopy with the SR dye molecules as optical probs. It is found that there are the anti-correlated characteristics to the orthogonal polarization of single molecules fluorescence when the SR molecules are absorbed onto the PMMA surface. It is presented directly that the rotational dynamics of the polymer surface is revealed by the cross-correlation function, and the rotational time is measurement. Accordingly, the molecules embedded inside the polymer film are restricted by the surrounded environment and have low rotational freedom degree.