A multistep synthetic procedure for preparing novel C-60-anchored two-armed poly(tert-butyl acrylate) was developed. First, two-armed poly(tert-butyl acrylate) bearing a malonate ester core with well-controlled molecular weight was synthesized through atom transfer radical polymerization. The effective Bingel reaction between C-60 and the well-defined polymer was then carried out to yield C60-anchored polymer. GPC, H-1 NMR, and UV-vis spectroscopy indicated that the C60-anchored polymer was a monosubstituted and 'closed' 6,6-ring-bridged methanofullerene derivative.