<p>π-Conjugated polymers constitute an important class of materials for photoelectronic applications. Among them, systems in which higher-order structures are deliberately controlled have attracted increasing attention; as such, structural regulation often leads to refined morphologies and enhanced photoelectronic and chiroptical functions. Poly(acetylene)s bearing optically active substituents are representative examples, as they commonly adopt helical conformations with a predominantly one-handed screw sense, driven by cooperative intramolecular interactions at the side chains. In a related manner, poly(aryleneethynylene)s can form helical architectures by adjusting the hydrophobic–hydrophilic balance between the main chain and side chains, with these conformations being stabilized by intramolecular hydrogen bonding, van der Waals interactions, and other noncovalent forces. In some systems, such structural regulation further promotes the formation of well-defined aggregated states. Moreover, poly(aryleneethynylene)s incorporating platinum complex moieties represent a distinctive subclass in which higher-order structures can be modulated through coordination chemistry. In these materials, the effective conjugation length and the resulting optical properties, including absorption and emission characteristics, are governed not only by the polymer backbone but also by the nature of the coordinating ligands, highlighting the versatility of π-conjugated polymers as platforms for structure–function engineering.</p>