The linker 2,5-di(4-pyridyl)thiazolo[5,4-d]thiazole (Dptztz), whose synthesis and structure is described here, was utilized together with benzene-1,3-dicarboxylate (isophthalate, 1,3-BDC2−) for the preparation of the two-dimensional coordination network [Zn(1,3-BDC)Dptztz]·DMF (DMF = dimethylformamide) via a solvothermal reaction. Compound [Zn(1,3-BDC)Dptztz]·DMF belongs to the class of coordination polymers with interdigitated structure (CIDs). The incorporated DMF solvent molecules can be removed through solvent exchange and evacuation such that the supramolecular 3D packing of the 2D networks retains porosity for CO2 adsorption in activated [Zn(1,3-BDC)Dptztz]. The first sorption study of a tztz-functionalized porous metal-organic framework material yields a BET surface of 417 m2/g calculated from the CO2 adsorption data. The heat of adsorption for CO2 exhibits a relative maximum with 27.7 kJ/mol at an adsorbed CO2 amount of about 4 cm3/g STP, which is interpreted as a gate-opening effect.