•Distinguishing gating and pore-opening actions of flexible adsorbents•Tuning energy barrier avoiding pore opening for molecular sieving•Molecular sieving CO2/N2 CO2/CH4•Role host-guest interaction at the moment Molecular sieving, relying on simple size exclusion mechanism, is ideal adsorptive separation. While guest diffusion are generally judged by pore/aperture molecule sizes, precise determ...