It is easy for chemical pigments produced from organic chemicals to disappear when exposed to light over time. Recently, structurally colored pigments produced by materials with high indices of refraction such as TiO2 or ZnS have attracted great attention. This study presents that CdS@SiO2 core-shell nanospheres were synthesized through a homogeneous deposition method followed with a modified Stober method and a calcination process. Colored film assembled by pigments shows low angle dependence with high stability against degradation under environmental factors. Moreover, the structural color of CdS@SiO2 arrays was bright and tunable according to the size without changing the overall material design. Compared with the conventional method, the addition of black substances in colloidal spheres is the generally used method to realize angle-independent structural coloration. However, black materials (such as carbon blacks and acetylene black) are not stable because of the high surface energy, and usually reunite together easily, and then lead to a nonuniform distribution and significant decrease in brightness. Thus, we report self-assembly colored films with great low angle dependence but not any black substances. Moreover, the refractive index of CdS is higher than generally used PS, PMMA, and SiO2, and the SiO2 shell is poisonless. CdS@SiO2 structurally colored films have promising nonbleaching pigments and have potential applications for displays, colorimetric sensors, colorful decoration, and pigments.