Abstract This account describes recent aspects of the polyketone-based synthesis of functional molecules. Polyketones are rope-like compounds that combine conformational flexibility with reaction diversity. Although natural-type polyketones, bearing a repeating 1,3-diketone sequence, are difficult to handle as synthetic components owing to complex tautomerism and rapid intramolecular cyclization, the recent development of 1,3- and 1,4-diketone hybrid sequences has enabled access to stable, discrete polyketones for further synthetic functionalization. Various molecular structures with functional properties can be generated from the polyketone chains through rope manipulations, such as bending and coiling. Herein, we introduce their synthesis and structures, focusing on the functionality derived from π-conjugation and metal ion coordination with polyketone derivatives, such as solid-state photo emission, metal-ion conduction, and adsorption.