Direct current (DC) power transmission systems have received great attention because it can easily integrate many types of renewable energies and have low energy loss in long-distance and large-capacity power transmission for electricity global sharing. Nanoparticles (NPs) have a positive effect on the insulation properties of polymers, but weak interaction between NPs and polymer matrix greatly decreases the effort of NPs on the enhancement of insulation properties, and thereby limits its engineering application. In this work, grafting strategy was used to link the modified NPs and polymer matrix to improve their interactions. Silica NPs (SiO2-NPs) were modified by 3-(methacrylyloxy) propyl-trimethoxysilane (MPS) to introduce highly active groups on the SiO2-NPs surface, followed by the pre-irradiated linear low-density polyethylene (LLDPE) being easily grafted onto the MPS modified SiO2-NPs (MPS-SiO2-NPs) in the melt blending process to obtain LLDPE-g-MPS-SiO2-NPs nanocomposites. Fourier-transform infrared (FT-IR) spectrum and X-ray photoelectron spectroscopy (XPS) confirm the successful incorporation of MPS into SiO2-NPs. Transmission electron microscopy (TEM) verifies that the modified SiO2-NPs exhibits more uniform distribution. The rheology result shows that the interaction between MPS-SiO2-NPs and LLDPE significantly improves. More importantly, the LLDPE-g-MPS-SiO2-NPs nanocomposites displays superior DC breakdown strength to that fabricated by conventional modification methods. When the addition of MPS-SiO2-NPs is 0.1 wt%, the highest DC breakdown strength values of 525 kV/mm and 372 kV/mm are obtained at 30 °C and 70 °C, respectively, and high DC breakdown strength can be well maintained in a wide loading range of NPs.