In this study, N-allylsuccinamic acid (NASA) was synthesized in a single step with a yield of 85%. Carboxylic acid containing NASA was characterized through Fourier transform infrared (FTIR) radiation and 1H-NMR and 13C-NMR analysis, and then it was used for synthesis of poly(2-hydroxylethyl methacrylate-co-N-allylsuccinamic acid) [p(HEMA-co-NASA)] hydrogels. The structure of the obtained pH-responsive p(HEMA-co-NASA) hydrogels were characterized with FTIR spectroscopy and scanning electron microscopy analysis, and their swelling characterization was carried out under different drug-release conditions. In the application step of the study, the hydrogels were used for the in vitro release of vitamin B12 and Rhodamine 6G, which were selected as model drugs. We determined that the hydrogels used as a drug-delivery matrix could release the drug they had absorbed under different release conditions (phosphate-buffered saline, 0.9% NaCl, and pH 1.2) at high rates for time periods of up to 24 h. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014, 131, 39660.