Single crystal X-ray diffraction (SCXRD) analysis provided detailed structural insights of [Cu23H4(SC7H7)18(PPh3)6] (Cu23) NC. The results reveal that Cu23 NC crystallizes within a triclinic crystal system, specifically adopting the space group P-1 (No. 2) (Table ). A thorough structural analysis unveils a unique arrangement of Cu atoms and ligands in the Cu23 NC that is unparalleled by any previously known analogous structural architectures and geometries. The distinctive structure diverges from the commonly observed core-shell architectural geometry. Instead, this NC is formed by the fusion of two [Cu12H2(SC7H7)7(PPh3)3] subunits (Figure ). This fusion process is mediated by the strategic sharing of a single Cu atom positioned at a vertex, along with four additional thiolate ligands, between the two subunits. This results in a novel and intricate configuration. The detailed analysis of the subunit's anatomy reveals that nine Cu atoms primarily adopt identical elongated square pyramidal geometries. These geometries are categorized as a Johnson solid (specifically J8) (Figure ). Within these structures, the head Cu atoms, positioned at the apex of the pentagonal bases, contributes to the fusion process, forming a bielongated square pyramidal geometry comprising seventeen Cu atoms (Figure ). This configuration resembles a sand timer, with two elongated square pyramids sharing a common base (Figure ). Within each elongated square pyramid geometry, we observed a notable distortion in the arrangement of Cu atoms in the cubic portion (Figure ). We identified a disordered arrangement of the two vertex Cu atoms, which ultimately distorts the four connected facets, causing an overall structural distortion. In the two regular facets, the average Cu-Cu distance is 2.6697 ± 0.0153 Å, indicating strong cuprophilic interactions (Figure ). 39 However, in the irregular facets, the average Cu-Cu distance increases to 3.1354 ± 0.0694 Å due to the disordered arrangement, causing the Cu atoms to be pulled outward from the elongated square pyramid geometries. A more detailed analysis revealed that the two regular facets are maintained in an ordered arrangement due to the support from additional Cu atoms attached to the structure. One of these facets is connected to additional Cu atoms, forming the pentagonal base. The other facet is stabilized by the attachment of antenna-like Cu3 units, which form triangular prism-like geometries (Figure ). The average distance between the Cu atoms in this antenna-like Cu3 unit is 2.6572 ± 0.0292 Å, and it maintains an average distance of 2.7117 ± 0.0435 Å from the cubic facet, both indicative of strong cuprophilic interactions. These precise measurements suggest robust interactions that contribute to the structural integrity of the facet. Conversely, the absence of these stabilizing Cu3 units on the opposite facet results in a lack of structural support, causing the Cu atoms to be arranged in a disordered manner. So, the presence of the Cu3 units is thus crucial for maintaining the ordered structure and preventing the deformation observed in the absence of these units.