This review summarizes molecular photofunctions based on molecular magnetism, i.e., spin angular momenta and orbital angular momenta. From the viewpoint of spin manipulations of photoexcited states, the development of fluorescent probes for detecting vitamin C is illustrated. Also, the proposal of molecular magneto-optical memory and the magneto-chiral dichroism of organic compounds are introduced, which have been achieved by the use of orbital angular momenta of aromatic conjugated systems. Thus, this review demonstrates that the photofunctions based on molecular magnetism can open up novel scientific fields and technologies.