Self-assembly of colloidal spheres is the most frequently used method for structural colors, but the chroma of the structural colors is usually so low that people cannot observe it under natural conditions. This paper presents a facile method for fabrications of vivid structural colors by doping carbon black into the self-assembly of colloidal polymer spheres and nanosilica particles. This approach can generate very gorgeous structural colors which can be very easily seen under natural conditions. The fabrication conditions for the self-assembly of composite dispersions of polymer/silica/carbon black were optimized to obtain colloidal crystals with vivid colors. Thus, robust mechanical properties, large-scale, and brilliant structural colors can guarantee the obtained crystal films to find practical applications, which are demonstrated by the fact that the successful applications of structural colors beautify the original simple and tedious surface of bamboo strand board (BSB).