Summary: We investigated the formation of thermoresponsive gold nanoparticle/poly(N‐isopropylacrylamide) (AuNP/PNIPAAm) core/shell hybrid structures by surface‐initiated, atom transfer radical polymerization (SI‐ATRP) in aqueous media and the effect of cross‐linking on the thermoresponsiveness of the AuNP/PNIPAAm hybrids. The disulfide containing an ATRP initiator was attached onto AuNPs and the monomer, NIPAAm, was polymerized from the surface of AuNPs in the absence or presence of a cross‐linker, ethylene diacrylate, in aqueous media at room temperature. The resulting brush‐type and cross‐linked AuNP/PNIPAAm hybrids were characterized by Fourier‐transform infrared spectroscopy, transmission electron microscopy, and variable temperature dynamic light scattering.