The invention discloses a method for preparing a large-area structural coloration pattern by ink-jet printing. According to the method, high-reflective-index monodisperse colloidal microspheres, a high-boiling additive, ethanol, glycerol, a surfactant, a defoamer, adhesive, a pH adjusting agent and deionized water are mixed, and ink obtained through ultrasonic dispersion is injected into an ink cartridge of an ink jet printer for printing. According to the method, the high-reflective-index monodisperse colloidal microspheres are evenly deposited on paper through a common ink jet printer, and a short-range order and long-range disordered microstructure is obtained; and due to the mutual effect of the nanometer microspheres with different grain diameters and light, the structural color pattern with different colors can be obtained, the preparation of the large-area structural color pattern is achieved, the method is high in expansibility, and the method has the wide application prospects on the aspects of the display, security and the like.