Cadmium sulfide was prepared by colloidal synthesis in methyl methacrylate (MMA). Europium and terbium salts were added to the colloidal solutions. Using MMA radical polymerization, we synthesized PMMA/CdS:Eu(III), PMMA/CdS:Tb(III), and PMMA/CdS:Eu(III):Tb(III) luminescent composites. Their luminescence is due to defects in the CdS crystals and the 5Dо → 7Fj and 5D4 → 7Fj electronic transitions of the Eu3+ and Tb3+ ions, respectively. It depends on the composition of the materials, complexation on the surface of the colloidal particles, heat treatment time during synthesis, excitation wavelength, and other factors.