In the?current study, two novel Knoevenagel condensation products of substituted napthofuran-2-carbaldehydes were designed, synthesized and characterized. In order to study the intermolecular interactions of title compounds, single crystals were grown?by slow evaporation solution growth technique at?room temperature and crystal structure has been determined by single crystal X-ray diffraction technique. Both the molecules?crystallize in the monoclinic centrosymmetric space group?P21/c?with one molecule in the asymmetric unit. In?compound?[4]?the molecules are connected via bifurcated C-H···O=C and C-H···N=C?H-bonds and van der Waals interactions forming a layered structure, whereas in compound?[5a]?the molecular conformation is stabilized via intramolecular C-H···O H-bond and molecule interacts with other molecule generated via 21-screw?via?bifurcated C-H···O=C along with C-H···N=C H-bonds, which are interacting with nitro- of other molecule generated via same symmetry operation, forming bifurcated C-H···O-N?H-bonds, which helps in formation of molecular sheet-like structure.Further, in order to understand the various types
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