At present, mitigating carbon emissions from energy production and industrial processes is more relevant than ever to limit climate change. The widespread implementation of carbon capture technologies requires the development of cost-effective and selective adsorbents with high CO2 capture capacity and low thermal recovery. Coal fly ash has been extensively studied as a raw material for the synthesis of low-cost zeolite-like adsorbents for CO2 capture. Laboratory tests for CO2 adsorption onto coal fly ash zeolites (CFAZ) reveal promising results, but detailed computational studies are required to clarify the applicability of these materials as CO2 adsorbents on a pilot and industrial scale. The present study provides results for the validation of a simulation model for the design of adsorption columns for CO2 capture on CFAZ based on the experimental equilibrium and dynamic adsorption on a laboratory scale. The simulations were performed using ProSim DAC dynamic adsorption software to study mass transfer and energy balance in the thermal swing adsorption mode and in the most widely operated adsorption unit configuration.