In this paper, an adsorbent composite called S-PEMR, which consists of electrolytic manganese residues (EMR)- silicate minerals-based polyacrylic acid-polyacrylamide double-network hydrogels, has been developed. The successful synthesis was confirmed by the characteristic peaks of COO, amide I, C=O, -CH2, C-N group vibration in FTIR spectra as well as amorphous carbon in XRD patterns. This composite tackles the issue of harnessing EMR, which consists of layered silicate minerals and additional elements. These elements have potential value but are difficult to be effectively and safely utilized. It was observed that the adsorption process agreed with the quasi-secondary model and the Langmuir isotherm, the adsorption process is controlled by a chemisorption mechanism with the occurrence of electron sharing or electron transfer (establishment of covalent bonds) between the S-PEMR and the adsorbate. The S-PEMR was found to be recyclable up to four times. In the initial experiment, the concentrations of Ni, Cu, Cd, and Pb in a natural wastewater were recorded as 645.84, 906.21, 378.15, and 8.29 ug/L, respectively. The composites used in the study exhibited high removal efficiency for Ni (42.06%), Cu (93.14%), Cd (89.68%), and Pb (77.02%). The S-PEMR can be recycled up to four times with only a moderate reduction in adsorption performance. The removal mechanism primarily involved chelation or coordination, ion exchange, functional groups containing elements such as O and N, as well as the interaction of Si-O and Al-O with the heavy metal ions. This research establishes S-PEMR as a highly effective adsorbent for removing harmful contaminants from water.