Organic materials that spontaneously order into specific architectures could significantly advance our ability to harvest solar energy. However, developing these materials in traditional ways is a tedious process. This project will integrate computer-aided design (CAD), synthesis, and characterization to make a transformative approach in ordered organic materials discovery. An Indiana University team will study packing interactions and develop CAD algorithms for organic architectures. The architectures will form by spontaneous interactions of molecular building blocks programmed with specific features that connect them with neighbors. Resulting architectures will be characterized with state-of-the-art microscopy at single molecule resolution. Those data will be used to improve the design algorithm to reliably predict two-dimensional packing and film growth on surfaces. This algorithm will be implemented as computer software to supersede experiment and thus allow vast speed-ups in the discovery of new organic materials for harvesting solar energy. This work will have a broad impact on many applications of organic materials through free distribution of the design software and through national scientific symposia. The project will also sponsor recruitment of under-represented groups to scientific research careers and outreach to engage high school students in nanoscience education, thus impacting the next generation of scientists.