Melanin influences light reflection and absorption and is known to be one of the elements producing structural color, such as that in the feathers of birds. In this study, we used polydopamine (PDA), an artificial melanin, as a light-absorbing material and examined in detail the effect of its composite method on the structural color. The following two composite methods were investigated using cerium(IV) oxide (CeO2) particles as a core particle: binary coassembly of CeO2 and PDA particles and unary assembly of CeO2@PDA core-shell particles. Although both methods dramatically improved the visibility of the structural color by suppressing the scattered light owing to the light absorption capability of the PDA, there was a difference in the particle arrangement, angle dependence of the structural color, and color tone change. By selecting the PDA composite method, the guidelines for providing high visibility and the desired structural color were presented.