The feasibility of the use of adsorbent-coated microchannels in temperature swing adsorption (TSA) processes for natural gas purification is investigated by analyzing fluid flow and heat and mass transfer within the monolithic structure containing microchannels. It is found that the operational difficulties in heating commonly used adsorbent beds for the TSA process, due to very low adsorbent thermal conductivity and void space within the bed, can be minimized by introducing the adsorbent as a thin layer coating the microchannel walls. The adsorption, desorption, cooling, and purge stage performances are enhanced by the sharp species and thermal waves in the microchannels. The overall performance of the TSA-based purification process in the present study is found to be competitive with existing PSA-based cycles, yielding similar or higher product purities and recoveries and at least an order of magnitude greater purification capacity. The energy requirement for the process is also found comparable with documented bed-based processes.