Silane coupling agent was used to introduce polymeric groups that was C=C onto the surface of nano-SiO2 particles by self-assembling technique. Then, in situ grafted polymerization was carried out between the functionalized particles and butyl methacrylate monomers under the action of an initiating agent to accomplish the surface modification of nano-SiO2. The effect of different reaction conditions on grafting percentage was studied, and analyses of FTIR, TEM, and TG-DTA results show that new organic chains were introduced onto the surface of nano-SiO2, and the dispersion stability of nano-SiO2 in THF was obviously improved.