The separation of ethane from ethylene is an important but challenging process in the chemical industry because of their similar physicochemical properties. Generally, the adsorbents for C2H6/C2H4 separation require an appropriate and relatively small aperture. Herein, we report two dynamic pillar-layered metal-organic frameworks (MOFs) BUT-111 and BUT-112 with isomorphic frameworks but different degrees of interpenetration for efficient C2H4 purification. The dynamic behavior makes both the activated MOFs exhibit ultramicropores and reversed order adsorption behavior for C2H6 and C2H4, which could obtain highly purified C2H4 in one step from the C2H6/C2H4 mixture. BUT-111 and BUT-112 could work in a wide temperature range, and with the decrease in temperature, the C2H6/C2H4 selectivity would increase. Moreover, the degree of interpenetration could be well controlled by the synthetic temperature, and the increase in the interpenetration degree of BUT-112 enhanced the C2H4 purification effectively.