The research on dielectric frequency response of oil-paper composite insulation modified by nanoparticles has been carried out in order to seek possible way to improve insulation properties thereof. Before and after nanoparticles being added, the dielectric frequency responses of oil-paper composite insulation with different moisture contents at different temperatures have been measured within the frequency from 0.1 mHz to 1 MHz. The Cole-Cole relaxation model has been used to analyzing the measured data. The results show that the variation rules of insulation condition can be indicated by the parameters of relaxation model. By adding nanoparticles, a new low frequency relaxation appeared.