The future of electronics, displays and lighting, large-area power generation and storage, and sensors for medical and national security applications requires the continued development of new materials to meet the ever more complex scientific and engineering challenges presented by these technologies. Carbon-based (organic) semiconductors offer opportunities to meet and even exceed the performance metrics required for these applications. However, many questions remain as to which organic semiconductors best fit each of these applications and how best to make them, as they themselves can be complex. To tackle these challenges and accelerate the commercial readiness of organic semiconductors, the ACROSS (Accelerating the Commercial Readiness of Organic Semiconductor Systems) team brings together expertise from chemistry, physics, device engineering, materials science, and modeling and data science to speed up applications-specific materials design. Notably, ACROSS provides a distinct, multidisciplinary environment to train the next generation of diverse and inquisitive scientists and engineers, where computers and machines will be vital to drive discovery.