Cu-MOF-74 (also known as Cu-CPO-27) was identified as a sorbent having one of the highest densities of Cu(II) sites per unit volume. Given that Cu(II) in the framework can be thermally activated to yield a five-coordinate Cu(II) species, we identified this MOF as a potential candidate for maximal volumetric uptake of ammonia. To that end, the kinetic breakthrough of ammonia in Cu-MOF-74/Cu-CPO-27 was examined under both dry and humid conditions. Under dry conditions the MOF exhibited a respectable performance (2.6 vs. 2.9 NH3 per nm3 for the current record holder HKUST-1), and under 80% relative humidity, the MOF outperformed HKUST-1 (5.9 vs. 3.9 NH3 per nm3, respectively).