Materials design has become a vigorous aspect for organic solid‐state lasing, which often lacks a fundamental understanding of structure–property relationships. The development of such an understanding is undertaken in this progress report, which systematically explores the now‐available libraries of organic single crystals exhibiting light amplification under optical pumping. By doing so, intra‐ and intermolecular contributions are disentangled for the non‐/occurrence, type, threshold, wavelength, and polarization of the light amplification processes, opening the path to targeted materials design.