The tunability of the colors and emissions of quantum-dot (QD) films—by controlling the deposition order and number of bilayers in (PDDA–CdSe@CdS)n and (PDDA–CdTe)n films (PDDA: poly(diallyldimethylammonium chloride))—is demonstrated. The photograph shows QD microstructures that exhibit different emission colors on a gold nanoparticle (AuNP)-treated indium tin oxide substrate, fabricated by combining layer-by-layer assembly with photolithography.