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This letter reports the role of nanoparticle surface modification in affecting the space charge distribution of polyethylene/silica nanocomposite dielectrics. Space charge distribution in the nanocomposites was measured using a pulsed electroacoustic method. The results suggested that the nanoparticle surface modification has significant effects on the space charge behaviors in polyethylene and that the nanocomposites with surface-treated silica showed improved space charge distribution, which can be understood in terms of the morphological variation of the matrix and the better interfacial adhesion between the surface-treated nanoparticles and the matrix.