This study presents the influence of various types of nanoparticle (NP) fillers incorporated into a polyurethane (PU) (VUKOL 022) matrix and its subsequent changes in complex permittivity. Two types of surface modification of SiO2 fillers were investigated. The frequency dependence of the real and imaginary parts of complex permittivity was measured within the frequency range of 1 mHz to 1 MHz using the capacitance method. The 1 wt.% NPs in PU caused an increase (MgO, TiO2, n-SiO2, and f-SiO2) or a decrease (d-SiO2) in the real permittivity. The $\alpha $ -relaxation and intermediate dipolar effect were observed at the temperature dependence of the imaginary permittivity. The change in permittivity by various surface modifications of SiO2 and other nanofillers was discussed based on the multi-core model. Moreover, the NPs caused a shift in the local maximum of the permittivity, which was a result of the interfacial polarisation and a charge multiplication of the $\alpha $ -relaxation process.