While there exist many hard-and-fast principles to manipulate at the atomic-scale the electronic, redox, and optical characteristics of π-conjugated molecules and polymers, the translation of these molecular characteristics to the macroscopic materials properties that are critical to the functionality of organic semiconductors remains highly Edisonian. Recent experimental and theoretical efforts have brought forward some under underpinnings to direct molecular-scale and microscopic order in organic semiconductors through molecular and process design, though these concepts are not robust and often fall short across materials classes. This workshop will bring together synthetic chemists, materials scientists and engineers, process design specialists, device engineers, and theoreticians to chart the next steps forward in the design of new generations of organic semiconductors with a view towards controlling assembly.