Novel polyaspartamide copolymers containing histamine pendants (PHEA‐HIS) were prepared from polysuccinimide, which is the thermal polycondensation product of aspartic acid, via a successive ring‐opening reaction using histamine (HIS) and ethanolamine (EA). The prepared water‐soluble copolymer was then crosslinked by reacting it with hexamethylene diisocyanate in order to provide a hydrogel with both good gel strength and reversible CO2 absorption characteristics. PHEA‐HIS gel is also pH‐sensitive and eligible to coordinate to metal ions such as Pb2+, Cu2+, and Ni2+ due to the imidazole units in its structure. The CO2‐responsive swelling behavior, metal‐ion adsorption, and morphology of the crosslinked gels were investigated. The approach described here results is a promising hydrogel with potential for a variety of industrial and biomedical applications including CO2 capture, CO2‐responsive and switchable sensors, and smart drug delivery systems. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016, 133, 43305.