Concomitant photoinduced magnetic and electrical phenomena are reported for the organic-based magnetic semiconductor V(TCNE)(x) (x similar to 2; TCNE=tetracyanoethylene; magnetic ordering temperature T-c similar to 400 K). Upon optical excitation (457.9 nm), the system can be trapped in a thermally reversible photoexcited state, which exhibits reduced magnetic susceptibility and increased conductivity with a simultaneous change in IR absorption spectrum. The multiple photonic effects in V(TCNE)(x) are proposed to originate from structural changes induced by internal excitation in (TCNE)(-) anions, which lead to relaxation to a long-lived metastable state.