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Polymer electrolytes are essential for next-generation lithium batteries because of their excellent safety record. However, low ionic conductivity is the main obstacle restricting their commercial application. Composites with nanoparticles are a promising route to overcome this obstacle. In this work, lithium polystyrene sulfonate brushes (LiPSS) is anchored to silicon dioxide nanoparticles with chemical bonding using atom transfer radial polymerization (SI-ATRP). The composite polymer electrolytes are made by mixing vinylene carbonate and nanoparticles via a facile in situ polymerization process. The ionic conductivity of composite polymer electrolytes is improved to 7.2 × 10-4 S/cm at room temperature, which is attributed to the low degree of crystallinity of polymer electrolyte and the fast ion transport on the surfaces of polymer brush layers that act as a conductive network. The composite polymer electrolytes show a wide electrochemical window of approximately 4.5 V vs. Li+/Li and excellent cycling performance retention of approximately 95％after 100 cycles at ambient temperature. The results also prove that surface groups of ceramic nanoparticles are an important way to increase the electrochemical properties of composite polymer electrolytes.