The modification of zeolite mining waste (ZMW) to develop a solid adsorbent for carbon dioxide (CO₂) capture presents significant potential for low-pressure CO₂ immobilization with a reduced carbon footprint, offering a sustainable alternative to conventional adsorbents such as metal-organic frameworks (MOFs). The dealumination process applied to ZMW produces materials with distinct mineral frameworks, significantly altering micropore concentration and surface morphology. Aluminium removal varies from 40.4% to 86.5%, corresponding to Si/Al ratios from 8.2 to 36.2. Lower dealumination conditions existing pores, while strong dealumination creates new pores and reduces external surface area. Intermediate aluminium removal results in surface polishing, low micropore area, and high external surface area. Monoethanolamine (MEA) impregnation is carried out using the wet impregnation method and confirmed by Fourier transform infrared spectroscopy (FTIR) and thermogravimetry (TG). The L16(3⁴) orthogonal experimental design identifies the optimal region for CO₂ uptake in relation to H₂SO₄ concentration, reaction time, and MEA loading. A 1% MEA loading provides the highest CO₂ uptake regardless of Si/Al ratio, indicating steric hindrance at higher loadings. FTIR confirms MEA on the zeolite surface and suggests adsorption and desorption below 99 °C to avoid degradation. These results support ZMW as a low-cost, low-carbon adsorbent for CO₂ capture.