We report an advanced method for the self-organization of an optomagnetic nanocomposite composed of both fluorescent clusters (ZnS quantum dots, QDs) and magnetic nanoparticles (CoFe2O4). ZnS nanocrystals were prepared via an aqueous method at different temperatures (25, 50, 75, and 100 °C). Their structural, optical and chemical properties were comprehensively characterized by X-ray diffraction (XRD), UV-Vis, photoluminescence (PL) spectroscopy, scanning electron microscopy (SEM), dynamic light scattering (DLS), transmission electron microscopy (TEM), and infrared spectroscopy (FT-IR). The highest PL intensity was observed for the cubic ZnS nanoparticles synthesized at 75 °C which were then stabilized electrosterically using thioglycolic acid. The photophysical analysis of the capped QDs with particle size in the range 9-25 nm revealed that the emission intensity increases and the optical band gap rises compared to uncapped nanocrystals (3.88 to 4.02 eV). These band gaps are both wider than that of bulk ZnS resulting from the quantum confinement effect. Magnetic nanoparticles were synthesized via a coprecipitation route and a sol-gel process was used to form the functionalized, silica-coated CoFe2O4. Finally, thiol coordination was used for binding the QDs to the surface of the magnetic nanoparticles. The fluorescence intensity and magnetic properties of the nanocomposites are related to the ratio of ZnS and CoFe2O4. As-prepared optomagnetic nanocomposite with small size (12-45 nm), acceptable saturation magnetization (about 6.7 emu/g), and satisfactory luminescent characteristics could be successfully prepared. These are promising candidates for biological and photocatalytic applications.