<p>Metal nanoclusters, particularly those bridging molecular and metallic states, play a crucial role in understanding the relationship between atomic structure and emergent physical properties. Herein we report the synthesis and crystal structure of Ag₁₃₅Cu₆₀(S(CH₂)₂Ph)₆₀Cl₄₂ (Ag₁₃₅Cu₆₀ for short hereafter; −S(CH₂)₂Ph = phenylethanethiolate), which contains an Ag₁₃₅ structure derived from the removal of twelve vertices from the 147-atom Mackay icosahedron, further wrapped by copper complexes. Ag₁₃₅Cu₆₀ was obtained via sodium borohydride reduction of a solution of AgCu-S(CH₂)₂Ph complexes, and it can be described as a core–shell metal cage Ag₁₃@Ag₄₂@Ag₆₀Ag₂₀@Cl₁₂@Cu₆₀ co-protected by −S(CH₂)₂Ph and Cl ligands. This shell-by-shell assembly leads to varying electron delocalization owing to changes in the length of metal–metal bonds, giving Ag₁₃₅Cu₆₀ both molecular and metallic properties leading to unusual power dependencies resulting from molecular-state-directed acoustic oscillations. This research inspires further exploration into customizable metal nanocluster structures and opens up opportunities to study the influence of nanocluster structure on the metallic state. The findings ultimately provide valuable insights for advancing the fields of nanotechnology and materials science, paving the way for innovative applications in developing advanced nanomaterials.</p><p></p>