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Hydrogels have been widely used for adsorbing heavy metal ions in wastewater treatment. Herein, a calcium alginate/poly‐N‐isopropylacrylamide double‐network hydrogel with photothermal responsiveness was prepared for adsorbing heavy metal ions in aqueous solution. The chemical composition, micromorphology, swelling properties, photothermal responsiveness, adsorption properties, and adsorption mechanism of gel microspheres were studied, respectively. The gel microspheres had an interpenetrating three‐dimensional porous structure, and their high porosity morphology and high specific surface area could ensure the adequate exposure of active adsorption sites. The gel microspheres showed excellent selective adsorption of Cr(III), and the theoretical maximum adsorption capacity of 146.16 mg/g was calculated according to the Langmuir model. Besides, its excellent photothermal conversion ability enhanced the resistance to external interference after the adsorption. Our work has provided an innovative approach to solar water purification while optimizing the preparation process. [ABSTRACT FROM AUTHOR]