CdTe nanocrystals capped with 1-mercapto-2,3-propandiol, CdSe nanocrystals capped with sodium citrate, and core−shell CdSe/CdS nanocrystals capped with sodium citrate were synthesized in aqueous solutions, and their surface was modified by 3-mercaptopropyltrimethoxysilane (MPS) in water−ethanol mixtures. By addition of sodium silicate, “raisin bun”-type composite particles were formed, with either CdTe, CdSe, or CdSe/CdS nanocrystals being homogeneously incorporated as multiple cores into silica spheres of 40−80 nm size, accompanied by some alteration of optical properties of the nanoparticles and, in particular, the reduction of the luminescence quantum yield. Further, growth of larger silica spheres (100−700 nm) can be performed by the Stober technique using either MPS-modified semiconductor nanocrystals or “raisin bun”-type composite particles as seeds, which gives semiconductor-doped silica globules of desirable sizes in the submicrometer range. The composite spheres can be used as building blocks for...