Two naphthalene (NP) and bipyridinium (BIPY2+) alternately incorporated polymers P1 and P2 have been prepared through the formation of dynamic hydrazone bonds. The polymers formed NP–BIPY2+ donor–acceptor interaction-induced pleated secondary structure. Upon reducing the BIPY2+ units to radical cation BIPY+, intramolecular dimerization of the BIPY+ units induced the backbones to afford another pleated secondary structure. Adding electron-rich macrocyclic polyether bis-1,5-dinaphtho[38]crown-10 or electron-deficient cyclobis(paraquat-p-phenylene) cyclophane did not break the first foldamer by complexing the BIPY2+ or NP units of the polymers, whereas the di(radical cationic) ring of the second cyclophane could break the second foldamer by forming threading complexes with the BIPY+ units of the polymers.