Affordable, low-cost flexible electronics will revolutionize how society thinks about and uses devices in applications ranging from energy storage and conversion, displays, or sensors for environmental and health monitoring. Conjugated polymers can provide the key functional component for electrical performance; however, control of the thin-film, active-layer morphology presents a key challenge. This project merges knowledge from polymer design, synthesis and processing, high-throughput combinatorial materials discovery, multiscale materials simulation, and materials informatics to stimulate the discovery of new generations of flexible, stretchable and high-temperature semiconductors enabled by blends of conjugated polymers and electrically inert polymers that exhibit unprecedented and robust performance.