Studies of photoinduced magnetization and photoinduced absorption in molecule-based magnet Mn(TCNE)x∙y(CH2Cl2) (x≈2, y∼0.8, TCNE=tetracyanoethylene) are reported. Optical excitation in the blue region of spectrum leads to increased magnetization, accompanied by changes in the electronic spectrum. These effects are preserved long after illumination, indicating formation of a highly metastable electronic state. Partial reversal of the photoinduced effects is obtained by excitation with lower energy visible light. The results suggest that the photoinduced effects are controlled by two distinct electronic transitions. © 2002 American Institute of Physics.