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A series of Co/Alq3 granular film samples are prepared using co-evaporating technique. The microstructures and magnetic properties are investigated. The Kerr spectra and optical constants of Cox(Alq3)1-x(0.19≤x＜1) granular films are measured using a magneto-optical Kerr spectrometer and a spectroscopic ellipsometer in the 1.5-4.5 eV photon energy range. The Kerr rotation reaches the maximum value of 0.5° in the x = 0.65 sample. The relationship between enhanced Kerr rotation and optical constants is discussed, and the concentration dependence of MOKE spectra is also investigated.