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 CO(2) capture ability.