Dry reforming of methane (DRM) involves the conversion of CO2 and CH4, the most important greenhouse gases, into syngas, a stoichiometric mixture of H2 and CO that can be further processed via Fischer–Tropsch chemistry into a wide variety of products. However, the devolvement of the coke resistant catalyst, especially at high pressures, is still hampering commercial applications. One of the relatively new approaches for the synthesis of metal nanoparticle based catalysts comprises the use of metal-organic frameworks (MOFs) as catalyst precursors. In this work we have explored MOF-74/CPO-27 MOFs as precursors for the synthesis of Ni, Co and bimetallic Ni-Co metal nanoparticles. Our results show that the bimetallic system produced through pyrolysis of a Ni-Co@CMOF-74 precursor displays the best activity at moderate pressures, with stable performance during at least 10 h at 700 ◦C, 5 bar and 33 L·h−1·g−1.