Smart hydrogels, or stimuli-responsive hydrogels, are three-dimensional networks composed of crosslinked hydrophilic polymer chains that are able to dramatically change their volume and other properties in response to environmental stimuli such as temperature, pH and certain chemicals. Rapid and significant response to environmental stimuli and high elasticity are critical for the versatility of such smart hydrogels. Here we report the synthesis of smart hydrogels which are rapidly responsive, highly swellable and stretchable, by constructing a nano-structured architecture with activated nanogels as nano-crosslinkers. The nano-structured smart hydrogels show very significant and rapid stimuli-responsive characteristics, as well as highly elastic properties to sustain high compressions, resist slicing and withstand high level of deformation, such as bending, twisting and extensive stretching. Because of the concurrent rapid and significant stimuli-response and high elasticity, these nano-structured smart hydrogels may expand the scope of hydrogel applications, and provide enhanced performance in their applications.