Wastewater is a by-product of numerous industrial processes that have been demonstrated to have adverse effects on human and natural health due to the pollutants it contains. The pollutants in these substances are organic or inorganic molecules and heavy metal ions that significantly harm the environment and human health. A variety of techniques have been devised for the removal of heavy metal ions from wastewater. The adsorption process has attracted significant attention due to its straightforward implementation, cost-effectiveness, and the environmentally friendly production of adsorbent materials using biocompatible substances. In this study, the removal of Cu2+ ions from wastewater was conducted using chitosan pullulan, a biocompatible and biodegradable polymer. In addition to chitosan and pullulan, waste refractory materials from a furnace used in iron and steel production were added to these polymer materials to increase the adsorption capacity. The initial step involved grinding the waste refractory brick material. Subsequently, chitosan was dissolved in acetic acid. After that, the refractory material was suspended in this solution, facilitating the formation of hydrogel beads using a NaOH solution. The obtained hydrogels were coated with pullulan to produce polyelectrolyte gel. Pullulan was oxidized to 6-carboxypullulan by the TEMPO (2,2,6,6-Tetramethylpiperidin-1-yl)oxyl) oxidation method and the negatively charged groups in its structure interacted with the positively charged groups in the chitosan structure to produce a complex gel. The chemical structure, morphological analysis, thermal analysis, and water release analysis of the produced waste refractory brick material added chitosan/oxidized pullulan complex gels were examined. The impact of the 6-carboxypullulan coating on the gels’ properties was elucidated. Furthermore, the adsorption of Cu2⁺ was conducted using solutions containing 100, 500, and 1000 ppm Cu2⁺ ions. It has been observed that the material can clean water with over 98% efficiency, even in solutions that exceed the standards set for wastewater. The material’s efficacy in cleaning solutions with concentrations above the standard for wastewater cleaning is evidence of its high performance. Furthermore, the kinetics and isotherm of the adsorption reaction were examined. The kinetics were determined to be consistent with the Pseudo Second Order (chemical reaction controlled) and aligned with the Langmuir and Freundlich Isotherm (mixed adsorption occurred on homogeneous and heterogeneous surfaces).