A new class of fluorinated polymers was prepared by radical ring‐opening homopolymerization of vinylcyclopropane monomers with a perfluorinated (CF2)nF chain (n = 6, 8, or 10). The polymers were in fact copolymers composed of 1,5‐linear and cyclobutane isomer units, the relative content of which depended on n. Surprisingly, they formed liquid‐crystalline mesophases (SmBd and/or SmAd), which was attributed to phase separation of the incompatible fluorocarbon and hydrocarbon components of the repeat unit.

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