One‐Size‐Fits‐All: A Universal Binding Site for Single‐Layer Metal Cluster Self‐Assembly

Abstract 2D metal clusters maximize atom–surface interactions, making them highly attractive for energy and electronic technologies. However, their fabrication remains extremely challenging because they are thermodynamically unstable. Current methods are limited to element‐specific binding sites or confinement of metals between layers, with no universal strategy achieved to date. Here, a general approach is presented that uses vacancy defects as universal binding sites to fabricate single‐layer metal clusters (SLMC). It is demonstrated that the density of these vacancies governs metal atom diffusion and bonding to the surface, overriding the metal's physicochemical properties. Crucially, the reactivity of vacancy sites must be preserved prior to metal deposition to enable SLMC formation. This strategy is demonstrated across 21 elements and their mixtures, yielding SLMC with areal densities up to 4.3 atoms∙nm⁻ ² , without heteroatom doping, while maintaining high thermal, environmental, and electrochemical stability. These findings provide a universal strategy for stabilizing SLMC, eliminating the need for element‐specific synthesis and metal confinement protocols and offering a strategy for efficiently utilizing metals.