We report a dynamical study on the photoinduced cooperative changes of the spin configurations in single crystals of the organometal spin-crossover complex. In the photoswitching process between low- and high-spin states, nonlinear characteristics such as thresholdlike behavior, incubation period, and phase separation have been observed. These results demonstrate that the cooperative intersystem crossing mediated by spin-lattice interaction plays a key role in the driving process of a new class of nonequilibrium phenomena so called photoinduced phase transition.