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The electrical properties of polymer nanocomposites are governed by the behavior of the internal charges. In particular, the interphase around the nanoparticles strongly influences the distribution and mobility of charge carriers within the nanocomposites, which, in turn, impacts the performance of these materials. In this work, we probe the internal charge behavior in the presence of nanoparticles with a focus on the low-frequency regime using a suite of techniques. By investigating the depolarizing currents and the dependence of the dielectric properties on the frequency and temperature, we demonstrate that the interphases redistribute the space charges, increase their trap depth, and suppress the electrode polarization in an elastomeric nanocomposite. Additionally, we study the effect of the nanoparticle content on the dielectric behavior by comparing the internal charge behavior of 1, 2, and 4 vol. % nanocomposites. At only 4 vol. % loading, the mobility of charge carriers is effectively limited, leading to lower dc conductivity compared to the unfilled elastomer, and 1 and 2 vol. % nanocomposites. These findings are based on the model materials used in this study, TiO2 nanoparticles and polydimethylsiloxane, and can be extended to other nanoparticulate-filled elastomer composites to design lightweight dielectrics, actuators, and sensors with improved capabilities. Judicious manipulation of interfacial phenomena in polymer nanocomposites—especially those with a dilute content of nanoparticles—provides a promising path forward for the design of materials with exceptional electrical and other physical properties.