Adsorption of Cu2+ and Co2+ from aqueous solution using zeolite synthesized from coal gangue was examined at room temperature. Batch experiments were carried out to investigate the effects of contact time, initial ion concentration, and pH on the adsorption process. Under comparable conditions, the adsorption greatly depended on initial ion concentration and pH. Different isotherms were applied to describe equilibrium data, and the results turned out that adsorption data can be better fitted with Langmuir, Temkin, and Dubinin–Radushkevich models, indicating monolayer coverage of adsorption sites on the surface of zeolite NaX and a physical process for Co2+ and Cu2+ adsorption. Adsorption capacity calculated from Langmuir was 45.05 mg/g for Cu2+ and 44.53 mg/g for Co2+. The adsorption kinetic could be better described with the pseudo-second-order model, and the removal mechanism of Co2+ and Cu2+ by the synthesized zeolite NaX was governed by surface adsorption, film diffusion, and intra-particle diffusion. The work suggests that coal gangue-derived zeolite NaX can be used as an alternative economical adsorbent for metal ions removal.