A novel macrogels poly(N,N-Dimethylacrylamide) (p(DMAAm)) and its derivatives were synthesized from DMAAm for use in urea uptake and release. p(DMAAm) surface was modified by NaOH and HCl to obtain p(DMAAm)/NaOH and p(DMAAm)/HCl, which are negatively and positively charged, respectively. The dynamic swelling behaviors, water retention and pH sensitivities of the macrogels were studied. It was found that all macrogels exhibited the equilibrium swelling ratio (SR) in the range 1068-1451%. Swelling kinetics showed that the macrogels possessed Fickian diffusion behavior while the diffusion coefficient of the macrogels varied from 1.41.10(-5) to 2.53.10(-5) cm(2)/min. Furthermore, urea uptake capacity and controlled release properties of the macrogels were studied. The maximum urea uptake capacity at pH 6 for p(DMAAm), p(DMAAm)/HCl, p(DMAAm)/NaOH macrogels were obtained to be 76.7 mg/g, 88.2 mg/g, 110.5 mg/g, respectively. It was concluded that the Langmuir isotherm fits quite well the experimental data. To describe the urea release kinetics, experimental data recorded at different pH solutions were computed through common release models. At pH 8, the p(DMAAm)/NaOH showed the highest release among the three prepared macrogel. Consequently, the results demonstrated that synthesized novel macrogels had high swelling rate and ability of absorbing and releasing of urea at different medium conditions.