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Polyisoprene-b-poly(ferrocenylmethylsilane) (PI-b-PFMS) copolymers, containing the atactic but semicrystalline PFMS block, have been prepared by sequential anionic polymerization of isoprene andmethylsilaferrocenophane. The reactionto formthemetalloblock isnot living in nature, but still enables three copolymers to be prepared (PI35-b-PFMS5, PI200-b-PFMS10, and PI247-b-PFMS23) with relative narrow molar mass distributions (polydispersity < 1.3). The self-assembly of all three materials is studied in PI selective n-alkanes and found to afford lenticular platelets, tapered cylindrical micelles, and regular cylinders, as the length of the PFMS block increased. PI200-b-PFMS10 micelles could be increased in length by self-seeding a sample of shortmicelles at temperatures of 90 C and above; however, this process also results in an increase in width. Addition of a solution of PI247-b-PFMS23 copolymer to preformed seed micelles also results in an increase in length, although growth is not linearly related to the amount of copolymer added beyond 600 nm.