The active layer of organic photovoltaic cells (OPVs) is typically a blend of p- and n-type semiconductors, and the arrangement of these materials largely affects the device performance. We have recently proposed a unique deposition technique in which α-diketone-type photoprecursors are solution-deposited and then subjected to in-situ photoreaction to form acene-based semiconductors, as an effective means for controlling the morphology and vertical composition profile in organic molecular blends. However, the applicability of this “photoprecursor approach” has been limited to p-type materials so far, restricting the flexibility in designing photovoltaic layers. Herein, we report α-diketone-type photoprecursors of two fullerene-anthracene co...