We believe that resolving the controversy around the role of solution aggregation requires probing the actual aggregate structure, which has been largely neglected in literature in part due to the analytical challenge. Besides, the evolution of solution aggregate structure during assembly has been mostly overlooked, which is a critical missing link between solution aggregation and solid-state properties . In sum, there is currently a gap in our knowledge regarding how to control the precise solution aggregate structures and assembly pathways of conjugated polymers, and how the solid-state morphology and electronic properties can be determined by different assembly pathways in a controllable fashion.