Despite many dedicated efforts, the fabrication of high-quality ZnO-incorporated Zinc@Silicon (Zn@Si) core–shell quantum dots (ZnSiQDs) with customized properties remains challenging. In this study, we report a new record for the brightness enhancement of ZnSiQDs prepared via a unified top-down and bottom-up strategy. The top-down approach was used to produce ZnSiQDs with uniform sizes and shapes, followed by the bottom-up method for their re-growth. The influence of various NH4OH contents (15 to 25 µL) on the morphology and optical characteristics of ZnSiQDs was investigated. The ZnSiQDs were obtained from the electrochemically etched porous Si (PSi) with Zn inclusion (ZnPSi), followed by the electropolishing and sonication in acetone. EFTEM micrographs of the samples prepared without and with NH4OH revealed the existence of spherical ZnSiQDs with a mean diameter of 1.22 to 7.4 nm, respectively. The emission spectra of the ZnSiQDs (excited by 365 nm) exhibited bright blue, green, orange-yellow, and red luminescence, indicating the uniform morphology related to the strong quantum confinement ZnSiQDs. In addition, the absorption and emission of the ZnSiQDs prepared with NH4OH were enhanced by 198.8% and 132.6%, respectively. The bandgap of the ZnSiQDs conditioned without and with NH4OH was approximately 3.6 and 2.3 eV, respectively.