The study of metallopolymers has blossomed into a mature field over the last few decades. Especially, polyferrocenylsilane (PFS) chemistry has taken a tremendous leap and continues to raise intense interest. Since the discovery of thermal ring-opening polymerization (ROP) of sila[1]ferrocenophanes, PFSs have been also accessed by anionic, cationic, transition-metal-catalyzed, and photolytic anionic ROP methodologies. A plethora of synthetic strategies have been devised, enabling access to a wide variety of copolymers, polyelectrolytes, and nanostructured materials. The distinctive physical properties and functions of many PFS-based polymers have been explored, leading to their apt exploitation in technical applications. Therefore, it is conceivable that PFS-related platforms might be indispensable nano-objects in the near future, as they stand on the verge of a new generation of sophisticated materials.

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Metallopolymere haben sich in den letzten Jahrzehnten zu einem ergiebigen Forschungsgebiet entwickelt. Besonders die Polyferrocenylsilan(PFS)‐Chemie hat sich dabei rasant entwickelt. Nach Entdeckung der thermischen Ringöffnungspolymerisation (ROP) von Sila[1]ferrocenophanen konnten Polyferrocenylsilane bald auch durch anionische, kationische, übergangsmetallkatalysierte und photolytische anionische ROP zugänglich gemacht werden. Hiervon ausgehend wurden unterschiedlichste weiterführende Synthesestrategien ausgearbeitet, die Zugang zu einer breiten Palette an Copolymeren, Polyelektrolyten und nanostrukturierten Materialien eröffnen. Die physikalischen Eigenschaften PFS‐basierter Polymere sowie die mit ihnen realisierbaren Funktionen wurden erforscht und können jetzt in technischen Anwendungen genutzt werden.

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Cover: Chemoselective stepwise coupling between living polymers and a heterobifunctional linking agent renders feasible the synthesis of block copolymers that are not accessible by sequential monomer addition. This facile and efficient synthetic tool resembles the versatility of a Swissarmy knife, being a powerful strategy for accessing welldefined block copolymers. Further details can be found in the article by V. Bellas, M. Rehahn on page 320.

Isothermal crystallization of the poly(ferrocenyl dimethylsilane) (PFDMS) segments in a poly[styrene‐block‐(ferrocenyl dimethylsilane)] (PS‐b‐PFDMS) diblock copolymer of lamellar micro‐morphology has been investigated. The PFDMS is shown to crystallize in a confined and grain‐by‐grain fashion. Here a ‘grain’ is defined as an ensemble of stacked lamellae wherein the PFDMS crystallization spreads quickly but stops at its surroundings. Such crystallization propagates not only along the PFDMS lamellae but across the amorphous PS layers as well. We suggest that conformational changes in the PS as induced by the PFDMS crystallization (‘squeezing transfer’) are responsible for the latter pathway of the crystallization's spread.