Structured adsorbents with high CO2 adsorption capacity, CO2 over N2 selectivity and rapid adsorption and desorption kinetics are ideal for CO2 capture from power-plant flue gas at a low cost. We report here binder-free zeolite monoliths with high CO2 over N2 selectivity (> 500) and uptake capacity (4mmolg-1) at 298 K and 101 kPa. Binder-free zeolite monoliths were consolidated by a rapid and facile processing approach called pulse current processing (PCP) from partially K exchanged NaA powders. The pore widow size of NaA was optimized by partially exchanging Na with K cations to achieve a high CO2 over N2 selectivity while maintaining a high CO2 uptake capacity. The CO2 uptake from binary mixtures of 0.10CO2-0.90N2 was obtained from the single component CO2 and N2 adsorption isotherms by applying Ideal adsorption solution (IAS) and Fast IAS theories. The binder-free adsorbents with an optimum degree of ion exchange display extraordinarily high CO2 over N2 selectivity and high CO2 uptake, together with a rapid CO2 adsorption and desorption kinetics and high mechanical stability. The performance of the new adsorbent has been compared with other potential candidates for efficient swing adsorption processes by a figure of merit. Key words: CO2 Capture; Zeolite monoliths; Pulse current processing; Selectivity; Adsorption; Ideal adsorbed solution (IAS) theory