Multiresponsive amphiphilic poly(N,N-dimethylaminoethyl methacrylate)-b-poly(Nisopropylacrylamide) (PDMAEMA-b-PNIPAM) was successfully synthesized by reversible addition-fragmentation chain transfer polymerization. Poly(N,Ndimethylaminoethyl methacrylate)-b-poly(N-isopropylacrylamide) has thermal and pH stimuli responsiveness. Their lower critical solution temperature and hydrodynamic radius can be adjusted by varying the copolymer composition, block length, solution pH, and temperature. In addition, a convenient method has been established to prepare cross-linked silica-coated nanoparticles with PDMAEMA-b-PNIPAM micelles as a template, resulting in good organic/inorganic hybrid nanoparticles defined as 175 to 220 nm. The structure and morphology were characterized by proton nuclear magnetic resonance ( 1 HNMR), Fourier-transform infrared spectroscopy (FT-IR), transmission electron microscopy (TEM), and transmission electron microscopy-energy dispersive X-ray spectroscopy (TEM-EDS).