pH-sensitive nanoclay composite hydrogels based on N-isopropylacryla-mide (NIPA) were synthesized by copolymerization with cationic and anionic comonomers. Laponite nanoclay particles served as multifunctional crosslinkers, producing hydrogels with exceptionally high mechanical strengths, as measured by elongation at break. Cationic copolymer gels based on NIPA and dimethylaminoethylmethacrylate were prepared by aqueous free radical polymerization, adopting a procedure reported by Harag-uchi (Adv Mater 2002, 14, 1120-1124). Without modification, this technique failed to produce anionic copolymer gels of NIPA and methacrylic acid (MAA), due to flocculation of clay particles. Three methods were conceived to incorporate acidic MAA into nanoclay hydrogels. First, NIPA was copolymerized with sodium methacrylate under dilute conditions, producing hydrogels with good pH-sensitivity but weak mechanical characteristics. Second, NIPA was copolymerized with methyl methacrylate, which was then hydrolyzed to generate acid sidegroups, yielding hydrogels that were much stronger but less pH sensitive. Third, NIPA was copolymerized with MAA following modification of the nanoclay surface with pyrophosphate ions. The resulting hydrogels exhibited both strong pH-sensitivities at 37 degrees C and excellent tensile properties. Optical transparency changed during polymerization, depending on hydrophobicity of the components. This work increases the diversity and functionality of nanoclay hydrogels, which display certain mechanical advantages over conventionally crosslinked hydrogels. (C) 2008 Wiley Periodicals, Inc.