Two pillared-layer metal-organic frameworks with pcu network were synthesized by the mechanochemical reaction of three components (ZnO, 3-amino-1,2,4-triazole (Harz) or 3,5-diamino-1,2,4-triazole (Hdatz), and isophthalic acid (H(2)ipa) at room temperature with space-time yield up to 4800 kgm(-3 )day(-1). The mechanochemically-synthesized [Zn-2(atz)(2)(ipa)] (Zn-atz-ipa) and [Zn-2(datz)(2)(ipa)] (Zn-datz-ipa) exhibit the high purity and porosity with BET surface areas of 655 and 572 m(2) g(-1) respectively, which are comparable with those synthesized by the traditional solvothermal method. In C2H4/C2H6 (v/v = 1/1) breakthrough experiment, Zn-datz-ipa can preferentially adsorb C2H6 over C2H4, showing a great potential for one-step purification of C2H4. In addition, this mechanochemical method can be scaled up to 100 mmol magnitude with single-pass production up to 20.0 g.