Satisfying mankind’s energy demand from sustainable sources is one of the key challenges of the 21st century. While Nature solved this challenge by harnessing solar energy with almost perfect efficiency, natural photosystems are highly complex, which limits their applications in artificial systems. We employ design and evolution to create efficient photobiocatalysts by equiping structurally simple – but catalytically proficient – heme-containing proteins with affordable organic photosensitizers. The resulting catalysts are employed to study photon-induced electron transfer and tailored for solar energy conversion and solar fuel production.