Nanocrystalline cellulose (NCC) whisker obtained from acid hydrolysis of cotton was incorporated into the freezing polymerized PNIPA/clay hydrogels to prepare inorganic–organic hybrid nanocomposite hydrogels (named as C-NC gels). The influence of NCC on the properties of C-NC gels was investigated systematically. It was found that all C-NC gels exhibit similar lower critical solution temperature as that of NCC-free gels, being independent of the NCC content. However, with the increase of NCC content in C-NC gels, the swelling ability of gels decreases slightly while the response rate of gels increases gradually, the gels with high content of NCC exhibit an ultrarapid deswelling rate due to the amount of interconnected micropores appeared inside the gels. Moreover, the enhancement effect of increased NCC on the gels is significant, which is also determined by the swelling degree of gels directly. Comparably, for the gels with the same content of NCC, higher strength was found when the gels were kept in lower swelling ratio due to the stronger interaction of NCC through hydrogen bond in the gels.
