Solubility plays a crucial role in the synthesis and application of conjugated polymers. It allows for processing of the polymers and fabrication of thin films, coatings, and electronic devices using solution-based techniques, such as spin coating or printing. For conjugated polymers, processability is normally achieved by attaching aliphatic side chains to the conjugated backbone that promote solubility in organic solvents. However, this approach is not without drawbacks. The introduction of aliphatic side chains can decrease the charge carrier mobility, reduce crystallinity, and alter the optical and electronic properties of the polymers, often necessitating tedious optimization of the side chain types and positions to balance solubility and desired performance characteristics. This can be rationalized by the fundamental role that side chains play in determining the polymer microstructure, with even minor structural or chemical changes having been shown to dramatically affect the assembly, ordering, and crystallinity of conjugated polymer thin films. Moreover, when conjugated polymers are used as organic battery electrode materials, the attachment of aliphatic side chains has a detrimental effect on the specific capacity, as the side chains increase the molecular weight without contributing to the capacity.