There is an increasing need for smart materials capable of removing multivalent ions from aqueous streams without the inconvenience of brine regeneration as in ionexchange processes.H erein, we present at hermoresponsive micellar system consisting of polystyrene-poly(methoxy diethyleneglycol acrylate) blockc opolymer surfactants modified with carboxylic acid end groups (PS-PMDEGA-COOH) that can be used to switchbetween the adsorption and desorption of divalent calcium(II) cations by amild temperature trigger,thus providing an ew type of thermoregenerable ion-adsorbing materials.T he switch of calcium(II)-binding capacity is demonstrated to result from as hift in the pK a value of the carboxylic acid groups by the collapse and redissolution of the PMDEGA blocka nd the associated change in local polarity.Hardness ions,such as calcium(II), cause problems in many processes by forming unwanted salt depositions.F or different applications,r anging from household applications,s uch as laundry and dish washing,t odrinking-water processes,t he softening of water streams is essential. [1,2] Thec urrent technology to bind multivalent ions is commonly based on the use of ion-exchange resins. [3,4] Ther egeneration of ionexchange resins typically involves consecutive washing steps involving brine or acid and caustic, thus leading to al arge amount of waste salt. [5,6] Thed isposal of these salts causes salinization of surface waters and soil, which is an increasing burden for the environment. Upcoming regenerate-disposal legislation has led several US states,s uch as California, to already install partial softener bans to deal with the salinization of surface waters.Therefore,the need for salt-free water softening is growing.Apromising approach is the use of smart polymer systems in which at hermal trigger is used as as witch between the adsorption and desorption of multivalent ions,s uch as calcium(II).[7] Af ew examples have been reported in which the lower critical solution temperature (LCST) of poly(Nisopropyl acrylamide) (PNIPAAm) is used to switch between adsorption and desorption.[8] However,most of these systems deal with ion adsorption at elevated temperatures (40-50 8 8C) and ion desorption at ambient temperature levels (10-20 8 8C) and are thus not practical for many applications,s ince ions often need to be adsorbed from natural water sources, generally found at ambient temperature levels.Furthermore, for systems based on athermal switch, it would be ideal to use wastewater streams with slightly elevated temperatures for regeneration.In the search for alternative ion-absorbing materials,w e have now developed am icellar system capable of adsorbing calcium(II) ions from water at ambient temperatures (10-20 8 8C) with the ability to desorb the bound ions at slightly elevated temperatures (40-50 8 8C). Low-grade waste heat can, thus,b eu sed to regenerate these micelles.T he micellar system is based on amphiphilic block-copolymer surfactants synthesized by atom-transfer radical polymerization (ATRP). Thes u...