Developing energy-effective alternatives for olefin/paraffin separations have been regarded as one of the most challenging separations in the petrochemical industry. In this work, a zinc-based pillar-layer metal-organic framework [Zn-2(5-aip)(2)(bpy)]center dot(DMF)center dot(H2O)(2) (1) is reported as a high-performance adsorbent for highly efficient separation of C3H6/C3H8 mixture. The structure and properties of 1 are confirmed by various characterization techniques. Then its adsorption and separation behaviors of C3H6 and C3H8 are systematically investigated. Although 1 has C3H6 adsorption capacity of 1.91 mmol/g at 100 kPa and 298 K, it exhibits preferential adsorption of C3H6 over C3H8 with high C3H6/C3H8 adsorption selectivity up to 19.8, outperforming most widely investigated MOFs. Furthermore, breakthrough experiments demonstrate that efficient separation of C3H6 over C3H8 on 1 can be achieved, revealing its outstanding separation performance under dynamic conditions. In particular, this material not only can be readily regenerated at 423 K within 20 min, but also exhibits good recyclability during five consecutive adsorption-desorption cycles. Thus, such advantages as high C3H6/C3H8 adsorption selectivity, easy regeneration and excellent recyclability make the pillar-layer 1 promising in practical application of C3H6/C3H8 separation.