Tangled cubes feature the topology of typical Platonic cubes, with their “faces” traversed by edges in different ways. This study generates an “A‐type” tangled metallocube from the reaction of binuclear gold‐NHC complex and H2S. The tangled cube topology was validated by multinuclear nuclear magnetic resonance (NMR) spectroscopy, high‐resolution electrospray‐ionization (HR‐ESI) mass spectrometry, and single‐crystal X‐ray diffraction analysis. This study offers a simple and effective approach to designing and fabricating new, topologically unique molecular structures. A molecular “A‐type” tangled metallocube has been generated by the reaction of a binuclear gold‐N‐heterocyclic carbene (NHC) complex and H2S. The tangled cube topology with 8 (μ3‐S)Au3+ units and 12 bis‐NHC ligands was validated by NMR spectroscopy, mass spectrometry, and single‐crystal X‐ray diffraction analysis.