The invention relates to a preparation and forming integrated three-dimensional printing method and a preparation and forming integrated three-dimensional printing device for amorphous alloy materials, belonging to the technical field of micro-droplet jetting material increase manufacturing and amorphous alloy preparation. Crystalline molten metal is directly jetted by using a metal droplet jetting material increase manufacturing technology; environmental cooling of a substrate before metal droplet jetting and deposition droplet cooling after the metal droplet jetting are realized by adopting a method of combining a rotatable double-jetting liquid nitrogen cooling device with a cold substrate; and by using a point-to-point cooling method for two times, the molten metal can be quenched and amorphized, and further the integration of preparation of the amorphous alloy materials and three-dimensional forming of a large-size complex structure are realized. According to the preparation and forming integrated three-dimensional printing method and the preparation and forming integrated three-dimensional printing device disclosed by the invention, the limit of a traditional preparation method of an amorphous alloy in a forming critical dimension of a bulk amorphous alloy is overcome; the defects of crystallization behavior and buckling deformation generated in the selective laser melting three-dimensional printing process of amorphous alloy powder are avoided; and the problem that the amorphous alloy materials are difficult to machine is solved, and the preparation and structure forming integrated three-dimensional printing of the amorphous alloy materials is realized.