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A versatile approach to fabricate nanoparticles with multiple functionalities through the combined use of both surface-initiated ATRP and acidolysis by H2S techniques was demonstrated. The hybrid nanoparticles exhibited the core-shell structure having the magnetite nanoparticles as the core and the polymethacrylate as the shell with PbS nanoparticles distributing in the shell. The structure and morphology of the synthesized nanoparticles were characterized using Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD) and transmission electron microscopy (TEM). The optical and magnetic properties of the nanoparticles were investigated by UV-Vis spectroscopy, photoluminescence spectroscopy and vibrating sample magnetometer (VSM), respectively. It is observed that the absorption and emission behaviors of the Fe3O4@PbS hybrid nanoparticles were seriously influenced by the ATRP time and the reaction time with H2S. The saturated magnetization (Ms) decreased with the increase of ATRP time due to the formation of thicker shells coating on the surfaces of magnetite nanoparticles.