Dendronized polyferrocenylsilanes were synthesized by a substitution reaction of reactive poly-(ferrocenylchloromethylsilane) with monodendrons with a focal hydroxy group. The resulting dendronized polymers were studied by H-1 NMR, differential scanning calorimetry (DSC), and polarized optical microscopy (POM). To facilitate the direct visualization of single polymer chains by atomic force microscopy (AFM), an interaction chromatography technique (IC) was used to fractionate the polydisperse polymers to separate the high molecular weight dendronized PFSs. AFM studies of the fractionated high molecular weight PFSs revealed a spherical cocoon for the single chains of the dendronized polymer as well as elongated single-chain structures. The cocoon of the dendronized PFS could be interesting as a unimolecular micelle with the transition-metal-rich core which is isolated by the dense outer layer of the dendrons.