In this work, a self-healing hydrogel has been prepared using in situ polymerization of acrylic acid and acrylamide in the presence of glycogen. The hydrogel was characterized using NMR, SEM, FT-IR, rheology, and dynamic light scattering (DLS) studies. The developed hydrogel exhibits self-healing properties at neutral pH, high swelling ability, high elasticity, and excellent mechanical strength. The hydrogel exhibits modulus values (G′, Ga″) as high as 106 Pa and shows an exceptionally high degree of swelling ratio (∼3.5 × 103). Further, the polymer based hydrogel adsorbs toxic metal ions (Cd2+, Pb2+, and Hg2+) and organic dyes (methylene blue and methyl orange) from contaminated water with remarkable efficiency (90-98%). The mechanistic analysis indicated the presence of pseudo-second-order reaction kinetics. The reusability of the hydrogel has been demonstrated by repeating the adsorption-desorption process over five cycles with identical results in the adsorption efficiency. (Graph Presented). © 2015 American Chemical Society.