We developed a facile but efficient method to grow tiny flowers of organometallic polymers along carbon nanotubes (CNTs), allowing the combination of synthesis and threading flowers onto CNTs in one step simultaneously. This afforded a catalog of redox-active tiny flower bundles of organometallic polymers with ultrathin petals. Crystallization of polyethylene end-functionalized with cyanoferrate complex (PE-Fe) along CNTs resulted in tiny flowers threaded onto CNTs. Subsequent coordination polymerization of surface-enriched cyanoferrate complex with Fe3+ afforded the formation of polyethylene/Prussian blue/carbon nanotube (PE-PB/CNT) hybrid flower bundles. The flowers were composed of thin petals of 7 nm in thickness, which consisted of a single PE lamellae sandwiched between two PB nanolayers. The hybrid flower bundles fabricated exhibited enhanced thermal stability and electrochemical activity. The intriguing microstructures along with morphology-related properties of hybrid flower bundles made them useful in nano devices and biosensors.