Atom‐precise nanoclusters‐metal‐organic framework (APNC/MOF) composites, as bifunctional material with well‐defined structures, have attracted considerable attention in recent years. Despite the progress made to date, there is an urgent need to develop a generic and scalable approach for all APNCs. Herein, the authors present the Exploiting Fracture Strategy (EFS) and successfully construct a super‐stable bifunctional APNC/ZIF‐8(300 °C) composite overcoming the limitations of previous strategies in selecting APNCs. The EFS utilizes the fracture of ZnN in ZIF‐8 after annealing at 300 °C. This method is suitable for all kinds of S/P protected APNCs with different sizes, including uncharged clusters Au1Ag39, Ag40, negatively charged Au12Ag32, positively charged Ag46Au24, Au4Cu4 and P‐ligand‐protected Pd3Cl. Importantly, the generated APNC/MOF show significantly improved performances, for example, the activities of Au12Ag32/ZIF‐8(300°C), Au4Cu4/ZIF‐8(300°C), and Au1Ag39/ZIF‐8(300°C) in the corresponding reactions are higher than those of Au12Ag32, Au4Cu4, and Au1Ag39, respectively. In particular, Au12Ag32/ZIF‐8(300 °C) shows higher activity than Au12Ag32@ZIF‐8. Therefore, this work offers guidance for the design of bifunctional APNC/MOF composites with excellent optimization of properties and opens up new horizons for future related nanomaterial studies and nanocatalyst designs.

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