Coal gangue and aluminum ash emerge as quintessential constituents within the ambit of coal-derived solid waste and industrial residue, respectively. Leveraging coal gangue as a primary substrate and aluminum ash as an adjunct aluminum source, molecular sieves can be synthesized through hydrothermal means. By modulating the dosage of aluminum ash, molecular sieves with varying crystalline structures can be obtained. The synthesized LTA-type molecular sieves manifest in two distinct morphologies: regular tetrahedral and stratified spherical stacking, evincing commendable Cu²⁺ adsorption efficacy. The Cu²⁺ adsorption phenomenon predominantly transpires via chemisorption, albeit with ancillary manifestations of physical adsorption. The valorization of coal gangue and aluminum ash towards the synthesis of molecular sieves not only underscores the elevation of industrial solid waste towards high-value utility, but also underscores the praxis of waste remediation through upcycling.