In this thesis, we studied the convenient synthesis and characterizations of thermo-responsive materials with double response. To achieve these, AB-type diblock copolymers comprising of poly(N-isopropylacrylamide) (NIPAAm) segment and poly(NIPAAm-co-(N-(hydroxymethyl)acrylamide) (HMAAm)) one were designed. That was synthesized in one-pot using an atom transfer radical polymerization (ATRP) technique. Poly(NIPAAm-co-HMAAm)s synthesized separately showed sensitive thermo-response and the cloud point was completely tunable by the composition of HMAAm. As expected, the block copolymers exhibited double thermo-responsive profiles in aqueous solution. The responsive behavior was discussed by precise trace by H-1 NMR and turbidity measurements. From these results, we could confirm almost independent dehydration of each segment. (C) 2008 Wiley Periodicals, Inc.