The gyroid is ubiquitous for underlying the construction of natural substance and artificial zeolites, but it has been, surprisingly, overlooked by chemists who work in the field of metal-organic frameworks (MOFs). In this work, a series of gyroidal MOFs with gie topology, constructed from 1,2-bis((5H-imidazol-4-yl)methylene)hydrazine and octahedral metal ions, such as Zn-II, Mn-II, Cu-II, and Ni-II, have been synthesized. The Zn-II analogue, named as STU-1, shows exceptional thermal and chemical stabilities, and exhibits permanent porosity and CO2 capture ability.