Electronic materials based on plastics possess unique optoelectronic and processing properties that provide exceptional opportunities for large-area lighting applications, novel versatile solar-energy harvesting platforms, next-generation sensors, future computing options, and beyond. If the development of plastic electronics systems can be accelerated, step changes will be achieved. For instance, new sustainable technologies may be produced that, e.g., integrate semi-transparent solar cells with greenhouses to yield a new class of sustainable, zero-energy, controlled-environment agriculture; assist with smart and controllable heat management for cars and office buildings; and/or allow the design of novel health-care devices. Despite extensive past efforts to further advance these materials and technology platforms, design- and processing- protocols remain based on trial-and-error methods, hampered by the highly intricate structure of plastic semiconductors, including complex structural dynamics. The critical bottleneck is that structure-function relations cannot be understood and categorized with classic nomenclature and classic approaches. New polymer physics and multi-disciplinary ML/AI approaches are proposed to be introduced to accelerate materials development.