The injection of CO2 into coalbed methane (CBM) reservoirs to enhance methane recovery has a second desirable benefit in simultaneously sequestering CO2. However, the real-time dynamic evolution of native adsorbed and rejected non-adsorbed methane during the process of CO2-enhanced coalbed methane (CO2-ECBM) production remains poorly constrained as a result of the nonlinear and hysteretic response of both CO2-CH4 interactions (part 1) and CO2-H2O wettability (part 2) of the coal under recreated reservoir conditions. In part 1, we apply calibrated nuclear magnetic resonance (NMR) to explore mechanisms of methane desorption and CO2 replacement during multiple cycles of CO2-ECBM flooding under recreated in situ conditions. Results for contrasting sub-bituminous coal and anthracite indicate that the adsorbed methane sweep efficiency is improved by similar to 16-26% with a single injection of CO2 over mere in situ desorption. Furthermore, CO2-CH4 displacement rates evolve during each CO2 injection cycle, first declining rapidly and then stabilizing with a long desorptive tail. Importantly, the cumulative methane sweep efficiency increases monotonically with successive cycles of CO2 injection, albeit at a reducing incremental efficiency, identifying the utility of cyclic CO2-ECBM as an effective method in both CO2 sequestration and enhanced gas recovery. Observed ratios of CO2 sorption capacities to CH4 recovery are 5.0 and 2.2 for sub-bituminous coal and anthracite, respectively, demonstrating an elevated potential for CO2 sequestration in sub-bituminous coals and more favorable CO2-ECBM recovery in anthracite, per unit mass of CO2 injected.