In this study, we demonstrated a new design technique for producing DNNH based on gellan-gum crosslinked by octavinyl polyhedral oligomeric silsesquioxane. Incorporating OV-POSS nanoparticles as cross-linkers into the first and second networks created strong coordination contacts and improved mechanical performance with 90% water. pH and contact time affect DNNH swelling, Ni(II), and Pb(II) removal. The resulting hydrogels were characterized by FT-IR, SEM, XRD, and TGA analyzes. The capacity of the hydrogel to adsorb Ni(II) and Pb(II) is 213.66 and 132.55 mg/g, respectively, according to the adsorption isotherm model. The usefulness of kinetic and isotherm investigations, notably the pseudo-second-order model and the Langmuir model, for the adsorption of the aforementioned contaminants, was proven. Ni(II) and Pb(II) adsorption is spontaneous and endothermic, according to the study. The hydrogel's adsorption-desorption reusability was renewed five times. As a consequence, the generated hydrogel is recognized as a good adsorbent for aqueous Ni(II) and Pb(II) adsorption.