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In this paper, the role of the accumulated surface charge on the surfaces of nanoparticles on breakdown strength for liquid and solid dielectrics is presented. The breakdown strengths of a nanofilled liquid dielectric and a solid dielectric are evaluated. The evaluation was conducted considering different nanoparticle material types with different nanofiller loadings. Accordingly, the preparation of transformer oil nanofluid and silicone rubber nanocomposites was performed with different nanofillers of the same average particle size. Breakdown voltage was measured for all the prepared samples, both liquid and solid. The interpretation of the obtained results is presented.