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Reaction of β-amino-β-(pyrid-4-yl)acrylonitrile with the aromatic dicarboxaldehydes 9,10-bis(4-formylphenyl)anthracene and terephthalaldehyde affords the dihydropyridyl products 9,10-bis(4-((3,5-dicyano-2,6-dipyridyl)dihydropyridyl)phenyl)anthracene (L¹) and 1,4-bis(4-(3,5-dicyano-2,6-dipyridyl)dihydropyridyl)benzene (L²), respectively. In the solid state [L¹]·2.5DMF·3MeOH (SOF-1) crystallizes in the monoclinic space group P2₁/c and forms a 3D stable supramolecular organic framework via strong N−H···N_py hydrogen bonds and π−π interactions. The material incorporates pyridyl-decorated channels and shows permanent porosity in the solid state. The pore volumes of the desolvated framework SOF-1a calculated from the N₂ isotherm at 125 K and the CO₂ isotherm at 195 K are 0.227 and 0.244 cm³ g⁻¹, respectively. The N₂ absorption capacity of SOF-1a at 77 K is very low, with an uptake of 0.63 mmol g⁻¹ …