Owing to their diverse physicochemical functions, conjugated polymers play a vital role in modern life and technology. One of the most important factors affecting the properties of conjugated polymers is their assembly structures. However, the rational design and control of polymer assemblies have yet to be optimized. In this focused review, strategies for regulating the assemblies of conjugated polymers at the molecular level using metal–organic frameworks (MOFs) are discussed. This methodology enables the elicitation of the unexplored properties of conjugated polymers as well as the fabrication of synergistic electronic nanohybrid materials.