1D Coordination Polymer (CP) of [Cu I (1,3-NCS)(DAFO)]n (CP1) (DAFO = 4,5-Diaza uoren-9-one) was synthesized using a branched tube method in ethanol and compared with previously synthesized CP2. Although the synthesis methods and parameters for CPs were di erent, both of them were formed in a similar crystal system (orthorhombic) and space group (P mn2 1 ) based on their X-ray crystallography data. Optical properties and structure of CP1 were further investigated in detail. Variation of the crystallography temperature causes slight di erences in the bond lengths and angles of the geometry center. Hirshfeld surface analyses show the signi cant contribution of H{C...H (18.9%) for CP1 and H{C...H (19.9%) for CP2. The most obvious distinctions between the CP interactions were C{N (8.4%) and (3.3%), Cu{S (4.8%) and (0.0%), and Cu{N (3.3%) and (11.4%) for CP1 and CP2, respectively. Non-Covalent Interaction-Reduced Density Gradient (NCI-RDG) analysis was conducted to broaden our understanding of the structure-directing interactions in these complexes. CP1 experienced signi cant inter-and intramolecular interactions according to Hirshfeld surface and NCI-RDG analyses. Solventfree decomposition of CP1 crystals at 750 C led to the synthesis of copper oxide (CuO) nanoparticles with a particle size of 12 nm.