Provided is a method of producing a metal-plastic multi-layered hybrid structure by using laser three-dimensional (3D) printing, the method including printing a metal structure on a substrate by using a first laser, patterning an upper surface of the metal structure by using the first laser, printing a polymer bonding layer on the patterned metal structure by using the first laser, and printing a polymer structure on the polymer bonding layer by using a second laser having a wavelength longer than a wavelength of the first laser, wherein the printing of the polymer bonding layer includes forming an intermediate phase at an interface between the metal structure and the polymer bonding layer. A layered structure produced using the above method may include the intermediate phase having the effect of an oxygen inclusion connecting a metal and a polymer.