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A facile and novel method for the fabrication of core-shell nanoparticles (PTMA@SiO2) based on a poly(2,2,6,6-tetramethylpiperidinyloxy-4-yl methacrylate) (PTMA) core and a porous SiO2 shell is reported. The core-shell nanoparticles are further self-assembled with negatively charged multi-walled carbon nanotubes (MWCNTs), which results in the formation of a free-standing cathode electrode. The porous SiO2 shell not only effectively improves the stability of the linear PTMA redox polymer with low molar mass in organic electrolytes but also leads to the uniform dispersion of PTMA active units in the MWCNTs conductive network. The PTMA@SiO2@MWCNT composite electrode exhibits a specific capacity as high as 73.8 mAh g at 1 C and only 0.11% capacity loss per cycle at a rate of 2 C.