CO2 and H2O diffusion in CALF-20 were studied with and without the presence of co-adsorbed N2 to determine the impact of N2 adsorption on the adsorption kinetics of H2O and CO2 in practical CO2 capture applications, where an abundance of N2 is present. This work showed that N2 has a measurable impact on the diffusion rate and mechanism of both CO2 and H2O in CALF-20. A new Fourier transform-based concentration swing frequency response method was used for the first time to collect the data to complete the measurements. Using multiple harmonics of the effluent response, multiple CSFR data points were collected with each experiment, reducing the measurement time by about threefold compared to conventional CSFR experiments. Overall, the FT-CSFR method provides rates that agree within a factor of 3 of CSFR rates collected using sine waves. The FT-CSFR method was validated by measuring single-component CO2 and H2O diffusion rates on CALF-20 at 4% CO2, and 5% and 40% RH, as well as MOF-303 at 10, 26, and 40% RH, as these conditions have been previously reported using sinusoidal CSFR. Binary CO2/N2 and H2O/N2 isotherms would be necessary for the full binary kinetic treatment of the CSFR data. However, applying the linear driving force model to the CO2/N2 system in a quasi-single component case appears to describe the behavior.